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  • kinetics  (727)
  • geochemistry
  • thema EDItEUR::T Technology, Engineering, Agriculture, Industrial processes::TN Civil engineering, surveying and building
  • Springer  (835)
  • FedOA - Federico II University Press  (2)
  • Digizeitschriften
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  • Moskva : Nauka
  • Wiley-Blackwell - STM
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  • 1
    Journal cover
    Unknown
    Moskva : Nauka
    Print: 1967 – 2000 (Location: A18, 3/2)
    Publisher: Moskva : Nauka
    Corporation: Akademija Nauk SSSR 〈Moskva〉 , Rossijskaja Akademija Nauk 〈Moskva〉
    Print ISSN: 0016-7525
    Topics: Geosciences
    Keywords: Geochemie ; geochemistry ; Russland
    Parallel titles: Геохимия , Geokhimia , Geokhimiya
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  • 2
    Journal cover
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    Wiley-Blackwell - STM | American Geophysical Union (AGU)
    Online: 1.2000 –
    Online: 1.2000 –
    Publisher: Wiley-Blackwell - STM , American Geophysical Union (AGU)
    Corporation: American Geophysical Union, AGU , Geochemical Society
    Electronic ISSN: 1525-2027
    Topics: Chemistry and Pharmacology , Geosciences , Physics
    Keywords: Geochemie ; geochemistry ; Geophysik ; geophysics ; United States of America ; USA
    Acronym: G-cubed
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  • 3
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    FedOA - Federico II University Press
    Publication Date: 2024-04-11
    Description: In the academic world, teaching is an educational experience that is not limited to the transfer of knowledge alone, but integrates with laboratory activities, especially in the training of building engineer or building-architect. In this way, each student has the opportunity to measure their aptitudes for design. The projects of socio-parish complexes, developed in the academic year 2021-2022, by the students of the Technical Architecture course, enrolled in the second year of the Building Engineering degree course at the University of Naples Federico II, are reported in this book. This work provides the opportunity to formulate reflections on laboratory teaching, in which the project is presented as a challenge launched by the teacher, shared by the tutors and taken up by the students. This "formative moment" was a strong, meaningful and engaging experience, until it converged into an exhibition set up at the parish of San Vitale Martire in Fuorigrotta, on 28 and 29 May 2022, on the occasion of the Festa dell'Approdo di San Paul. To the gratification of all the authors, the possibility of the citizens of the entire district of Fuorigrotta was added, the academic work taking it outside the university environments.
    Description: Published
    Description: La didattica nella realtà accademica è un’esperienza formativa che non si limita al trasferimento di conoscenze, ma, specialmente nella formazione dell’ingegnere edile o edile-architetto, si integra con la cosiddetta didattica laboratoriale, in cui ogni studente ha l’occasione di misurare le proprie attitudini alla progettazione. Questo lavoro, nel raccogliere progetti di complessi socio-parrocchiali, sviluppati dagli allievi della cattedra di Architettura Tecnica, iscritti al secondo anno del corso di laurea Ingegneria Edile-Architettura dell’Università di Napoli Federico II, nell’anno accademico 2021-2022, fornisce l’occasione di formulare riflessioni sulla didattica laboratoriale, in cui il progetto si pone come una vera e propria sfida lanciata dal docente, condivisa dai tutor e raccolta dagli allievi. Questo “momento formativo” è stata un’esperienza forte, pregnante e coinvolgente, fino a confluire in una mostra allestita presso la parrocchia di San Vitale Martire a Fuorigrotta ,nei giorni 28 e 29 maggio 2022, in occasione della Festa dell’Approdo di San Paolo. Alla gratificazione di tutti gli attori, si è aggiunta la possibilità di condividere con i cittadini dell’intera circoscrizione di Fuorigrotta, il lavoro accademico portandolo fuori dalle mura dell’Università.
    Keywords: socio-parish complexes ; laboratory teaching ; technical architecture ; eco-sustainable project ; social spaces ; thema EDItEUR::T Technology, Engineering, Agriculture, Industrial processes::TN Civil engineering, surveying and building
    Language: Italian
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  • 4
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    FedOA - Federico II University Press
    Publication Date: 2024-04-11
    Description: The volume collects the results of the Final Synthesis Laboratory coordinated by prof. Marella Santangelo, held in the academic year 2019/2020 as part of the fifth year of the DiARC degree course in Architecture of the University of Naples "Federico II". The students were confronted with the project of new spaces for the Secondigliano detention center in Naples. The laboratory was a space for experimentation around a complex architecture, with the aim of improving the quality of the places where the life of the prisoners takes place, but also of the different users of the prison building. In the first part, the teachers of the laboratory describe the way in which each discipline contributed to the development of the proposed theme. The second part presents the projects developed by the students recognizing three fundamental issues for the project of the spaces of the sentence: the knowledge of the functioning of the prison and its context, the way in which the architectural project can restore a public dimension to the Detention Center and finally, the importance of the spaces dedicated to the emotional relationships between prisoners and free people. The third part collects the contributions of personalities related to the prison world who interacted with the students during the course.
    Description: Published
    Description: Il volume restituisce gli esiti del Laboratorio di Sintesi Finale coordinato dalla prof. Marella Santangelo, svoltosi nell’anno accademico 2019/2020 nell’ambito del quinto anno del corso di Laurea magistrale in Architettura del DiARC dell’Università degli Studi di Napoli “Federico II”. Gli studenti si sono confrontati con il progetto di nuovi spazi per il centro penitenziario di Secondigliano a Napoli. Il laboratorio è stato uno spazio di sperimentazione intorno a un’architettura complessa, con l’obiettivo del miglioramento della qualità dei luoghi dove si svolge la vita dei detenuti, ma anche dei diversi utenti dell’edificio carcere. Nella prima parte i docenti del laboratorio descrivono il modo in cui ogni disciplina ha contribuito allo svolgimento del tema proposto. La seconda parte presenta i progetti sviluppati dagli studenti riconoscendo tre questioni fondamentali per il progetto degli spazi della pena: la conoscenza del funzionamento del carcere e del suo contesto, il modo in cui il progetto di architettura può restituire una dimensione pubblica all’Istituto Penitenziario e, infine, l’importanza degli spazi dedicati alle relazioni affettive tra detenuti e persone libere. La terza parte raccoglie i contributi di personalità legate al mondo del carcere che hanno interagito con gli studenti durante il corso.
    Keywords: Secondigliano ; architecture ; prison ; space ; detention ; thema EDItEUR::T Technology, Engineering, Agriculture, Industrial processes::TN Civil engineering, surveying and building
    Language: Italian
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  • 5
    Publication Date: 2021-07-13
    Description: The aim of this study was to investigate the microbial community thriving at two shallow hydrothermal vents off Panarea Island (Italy). Physico-chemical characteristics of thermal waters were examined in order to establish the effect of the vents on biodiversity of both Bacteria and Archaea. Water and adjacent sediment samples were collected at different times from two vents, characterised by different depth and temperature, and analysed to evaluate total microbial abundances, sulphuroxidising and thermophilic aerobic bacteria. Total microbial abundances were on average of the order of 105 cells ml-1, expressed as picoplanktonic size fraction. Picophytoplanktonic cells accounted for 0.77–3.83% of the total picoplanktonic cells. The contribution of bacterial and archaeal taxa to prokaryotic community diversity was investigated by PCR–DGGE fingerprinting method. The number of bands derived from bacterial DNA was highest in the DGGE profiles of water sample from the warmest and deepest site (site 2). In contrast, archaeal richness was highest in the water of the coldest and shallowest site (site 1). Sulphur-oxidising bacteria were detected by both culture- dependent and -independent methods. The primary production at the shallow hydrothermal system of Panarea is supported by a complex microbial community composed by phototrophs and chemolithotrophs.
    Description: Published
    Description: 199-212
    Description: 1.2. TTC - Sorveglianza geochimica delle aree vulcaniche attive
    Description: JCR Journal
    Description: reserved
    Keywords: hydrothermal vents ; bacteria ; geochemistry ; fluids ; 03. Hydrosphere::03.03. Physical::03.03.01. Air/water/earth interactions
    Repository Name: Istituto Nazionale di Geofisica e Vulcanologia (INGV)
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  • 6
    Publication Date: 2020-11-12
    Description: Fluid geochemistry monitoring in the Azores involves the regular sampling and analysis of gas discharges from fumaroles and measurements of CO2 diffuse soil gas emissions. Main degassing areas under monitoring are associated with hydrothermal systems of active central volcanoes in S. Miguel, Terceira and Graciosa islands. Fumarole discharge analysis since 1991 show that apart from steam these gas emissions are CO2 dominated with H2S, H2, CH4 and N2 in minor amounts. Mapping of CO2 diffuse soil emissions in S. Miguel Island lead to the conclusion that some inhabited areas are located within hazard-zones. At Furnas village, inside Furnas volcano caldera, about 62% of the 896 houses are within the CO2 anomaly, 5% being in areas of moderate to high risk. At Ribeira Seca, on the north flank of Fogo volcano, few family houses were evacuated when CO2 concentrations in the air reached 8 mol%. To assess and analyse the CO2 soil flux emissions, continuous monitoring stations were installed in S. Miguel (2), Terceira and Graciosa islands. The statistical analysis of the data showed that some meteorological parameters influence the CO2 flux. The average of CO2 flux in S. Miguel stations ranges from 250 g/m2/d at Furnas volcano to 530 g/m2/d at Fogo volcano. At Terceira Island it is about 330 g/m2/d and at Graciosa 4400 g/m2/d.
    Description: Published
    Description: JCR Journal
    Description: open
    Keywords: volcanology ; geochemistry ; soil degassing ; monitoring ; risk ; 04. Solid Earth::04.08. Volcanology::04.08.01. Gases ; 04. Solid Earth::04.08. Volcanology::04.08.06. Volcano monitoring
    Repository Name: Istituto Nazionale di Geofisica e Vulcanologia (INGV)
    Type: article
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  • 7
    Publication Date: 2019-11-04
    Description: Radon-in-soil monitoring at the Poas volcano (Costa Rica) has been performed together with water chemistry from the hot crater lake since 1981 and 1983 respectively. The results are discussed as a function of the eruptive evolution of the volcano over a 13 years period (1981-1994). It is shown that no definitely clear precursory radon signals have been recorded. On the contrary, ionic species concentrations are likely to be considered good precursors, together with the temperature variations of the crater lake water.
    Description: Published
    Description: JCR Journal
    Description: open
    Keywords: Poas volcano ; geochemistry ; radon ; precursor ; 04. Solid Earth::04.04. Geology::04.04.12. Fluid Geochemistry
    Repository Name: Istituto Nazionale di Geofisica e Vulcanologia (INGV)
    Type: article
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  • 8
    ISSN: 1539-6924
    Keywords: compliance certification application ; engineering analysis ; geochemistry ; geohydrology ; performance assessment ; probabilistic systems analysis ; radioactive waste ; scientific validity ; uncertainty ; 40 CFR 191
    Source: Springer Online Journal Archives 1860-2000
    Topics: Energy, Environment Protection, Nuclear Power Engineering
    Notes: Abstract Performance Assessment (PA) is the use of mathematical models to simulate the long-term behavior of engineered and geologic barriers in a nuclear waste repository; methods of uncertainty analysis are used to assess effects of parametric and conceptual uncertainties associated with the model system upon the uncertainty in outcomes of the simulation. PA is required by the U.S. Environmental Protection Agency as part of its certification process for geologic repositories for nuclear waste. This paper is a dialogue to explore the value and limitations of PA. Two “skeptics” acknowledge the utility of PA in organizing the scientific investigations that are necessary for confident siting and licensing of a repository; however, they maintain that the PA process, at least as it is currently implemented, is an essentially unscientific process with shortcomings that may provide results of limited use in evaluating actual effects on public health and safety. Conceptual uncertainties in a PA analysis can be so great that results can be confidently applied only over short time ranges, the antithesis of the purpose behind long-term, geologic disposal. Two “proponents” of PA agree that performance assessment is unscientific, but only in the sense that PA is an engineering analysis that uses existing scientific knowledge to support public policy decisions, rather than an investigation intended to increase fundamental knowledge of nature; PA has different goals and constraints than a typical scientific study. The “proponents” describe an ideal, six-step process for conducting generalized PA, here called probabilistic systems analysis (PSA); they note that virtually all scientific content of a PA is introduced during the model-building steps of a PSA; they contend that a PA based on simple but scientifically acceptable mathematical models can provide useful and objective input to regulatory decision makers. The value of the results of any PA must lie between these two views and will depend on the level of knowledge of the site, the degree to which models capture actual physical and chemical processes, the time over which extrapolations are made, and the proper evaluation of health risks attending implementation of the repository. The challenge is in evaluating whether the quality of the PA matches the needs of decision makers charged with protecting the health and safety of the public.
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  • 9
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    European journal of nutrition 26 (1987), S. 125-137 
    ISSN: 1436-6215
    Keywords: vitamin C ; functions ; kinetics ; pool ; saturation ; requirements ; RDA
    Source: Springer Online Journal Archives 1860-2000
    Topics: Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition , Medicine
    Description / Table of Contents: Zusammenfassung Die Bedeutung von Vitamin C für den menschlichen Organismus wird aus den wichtigen Funktionen ersichtlich, an denen das Vitamin beteiligt ist, wie zum Beispiel Kollagen- und Karnitinsynthesen. In neuerer Zeit entdeckt wurde seine Rolle bei der Noradrenalinsynthese, der Inaktivierung von freien Radikalen sowie der Verhinderung der Nitrosaminbildung. Die Vielfalt dieser Vitamin-C-abhängigen Funktionen läßt erkennen, daß die Bedarfsfestsetzung für Vitamin C nicht nur die Verhütung der Mangelkrankheit Skorbut anvisieren, sondern auch berücksichtigen sollte, daß alle diese Funktionen jederzeit genügend Vitamin C zur Verfügung haben müßten, um optimal reagieren zu können. Das Konzept der Gewebesättigung kommt diesem Ziel am nächsten. Studien mit einem kinetischen Modell haben ergeben, daß eine Sättigung mit täglicher Einnahme von 100 mg Vitamin C bei Nichtrauchern und von 140 mg bei Rauchern eintritt, Mengen, die als optimale Werte gelten können. Bei verschiedenen Krankheiten dürfte der Bedarf höher sein; die genauen Mengen müssen jedoch erst noch ermittelt werden.
    Notes: Summary The importance of vitamin C is reflected in its multifunctional roles which include participation in collagen and carnitine syntheses, promotion of iron absorption and the more recently discovered participation in noradrenaline synthesis, inactivation of free radical chain reactions, prevention of N-nitroso compound formation and more. Given the many extra-antiscorbutic functions of the vitamin, the Recommended Dietary Allowances (RDA) should not just prevent deficiency disease but should aim at providing sufficient amounts for all vitamin C-dependent functions to operate at full capacity. The concept of vitamin C tissue saturation is best able to meet this demand. The use of kinetic models has shown that the body pool is saturated with a daily intake of 100 mg vitamin C in non-smokers and 140 mg in smokers, amounts that may be regarded as optimal RDA values. Certain disease states may be accompanied by still higher vitamin C requirements but the exact amounts are not yet known.
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  • 10
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    Colloid & polymer science 261 (1983), S. 188-189 
    ISSN: 1435-1536
    Keywords: Polymerization ; kinetics ; redox polymerization ; acrylamide
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
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  • 11
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    Colloid & polymer science 266 (1988), S. 958-964 
    ISSN: 1435-1536
    Keywords: a-Se colloids ; photoadsorption ; kinetics ; activation energy ; compensation effect
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
    Notes: Abstract In this study, a model is developed to explain in microscopic terms the results obtained from thermally activated photoadsorption experiments in a-Se colloids. The observed compensation effect can be described for two different cases. At low efficiency adsorption, the process is controlled by the potential at the boundary layer. In the high efficiency adsorption case, the process is controlled by diffusion transport.
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  • 12
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    Colloid & polymer science 262 (1984), S. 366-373 
    ISSN: 1435-1536
    Keywords: kinetics ; isothermal crystallization ; polymer ; spherulite ; differential scanning calorimetry
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
    Notes: Abstract In the DSC technique, isothermal crystallization experiments are usually performed on thin flat specimens, but their interpretation generally uses theories developed for an unbounded volume. In this paper, isothermal crystallization of spherical entities in the volume limited by two parallel infinite planes is considered. Our model, derived from Avrami's theory, gives an analytical expression for the transformed volume fraction as a function of time. It is shown that the influence of thickness becomes important when thickness becomes of the order of or smaller than the average spherulite radius. The main effects of a decreasing thickness are a slower crystallization kinetics and a decrease in the Avrami exponent. These results can be used to interpret experimental data obtained in isothermal polymer crystallization.
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  • 13
    ISSN: 1435-1536
    Keywords: Phospholipid bilayer ; kinetics ; laser temperature jump ; phase transition
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
    Notes: Abstract The iodine-laser temperature-jump technique has been used to investigate the main phase transition in single shell vesicles of dimyristoylphosphatidylcholine. The probe molecules DPH and TMA-DPH were incorporated into the lipid bilayer and laserT-jump experiments with turbidity and flourescence polarization detection were performed. We found three well separated relaxation processes between 5 μs and 10 ms. The relaxation signals showed strong cooperativity in the relaxation times as well as in their corresponding amplituedes. We attributed the relaxation to the formation and dissolution of clusters of different order inside the bilayer.
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  • 14
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    Colloid & polymer science 265 (1987), S. 58-64 
    ISSN: 1435-1536
    Keywords: Polymerisation ; emulsion ; styrene ; methylmethacrylate ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
    Notes: Abstract The dependence of emulsion polymerisation rates on a number of important parameters is considered. Attention is paid to the use of seeded emulsion systems for the evaluation of radical desorption coefficients (k o). Experimental conditions are shown to be important. When the average number of radicals per particle is low, large changes in the rate coefficient for chain termination do not have a large effect on the kinetics. With styrene and methylmethacrylate, radical re-absorption by the polymer particles is shown to be important and radical capture efficiences can be high. Consistency is established between the results of a number of workers and values fork o are shown to be lower than those calculated from chain transfer rates.
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  • 15
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    Colloid & polymer science 261 (1983), S. 621-625 
    ISSN: 1435-1536
    Keywords: Polyamide 6 ; crystallisation ; kinetics ; titania
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
    Notes: Abstract The kinetics of isothermal and nonisothermal crystallization of polyamide-6 (PA6) containing titania was studied by means of DSC. It was found thatTiO 2 causes an acceleration in the crystallization of polyamide-6 and lowers the value of the Avrami exponent,n. The presence of TiO2 does not affect equilibrium melting pointT m 0 , glass temperatureT g, or surface free energiesσ e andσ of the basal and lateral surfaces.
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  • 16
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    Fire technology 20 (1984), S. 47-63 
    ISSN: 1572-8099
    Keywords: Extinguishment ; fire modeling ; mass loss ; heat release ; char ; reflash ; sprinklers ; radiant flux ; kinetics ; reaction rate ; heat loss ; ash ; latent heat ; spray density ; extinguishing agents
    Source: Springer Online Journal Archives 1860-2000
    Topics: Architecture, Civil Engineering, Surveying
    Notes: Abstract The Ad Hoc Mathematical Fire Modeling Working Group was organized about seven years ago to facilitate voluntary cooperation and coordination in developing mathematical fire modeling capability. The group has a steering committee of representatives of agencies that support fire modeling and related research. These include the National Bureau of Standards' Center for Fire Research, Factory Mutual Research Corp., the Naval Research Laboratory, NASA, and the Federal Aviation Agency. The Group holds plenary meetings when it seems desirable to do so (about once each 1 1/2 years), and workshops on topical subjects. Three workshops were held in 1983. Normally, Group meetings are held before or after other meetings at which a number of interested personnel would likely be present. Minutes are mailed to those who attended and to others (including European and Japanese personnel) who have indicated interest. This workshop was arranged by Ron Alpert of Factory Mutual Research Corp. and held at their facilities at Norwood, MA, in November 1983.
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  • 17
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    Journal of solution chemistry 11 (1982), S. 339-346 
    ISSN: 1572-8927
    Keywords: Carbon dioxide ; hydrolysis ; aqueous solution ; kinetics ; activation volume
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The pressure dependence of the dehydration reaction of H2CO3 was measured in acidic aqueous solution for pressures up to 1 kbar using a high-pressure stopped-flow instrument. The corresponding volume of activation was found to be 6.4±0.4 cm3-mol−1 at 25°C and 0.5 ionic strength. Volume equation calculations result in a value of −9.9±1.9cm3-mol−1 for the volume of activation for the hydrolysis of CO2 under the same conditions. For the first time, the reaction mechanism can be interpreted in terms of dissociative and associative modes, respectively. These data are used to construct an overall reaction volume profile.
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  • 18
    ISSN: 1572-8927
    Keywords: Temperature jump ; kinetics ; thermodynamics ; TRIS ; iminodiacetic acid ; magnesium ion ; phenol red
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Equations describing the temperature jump amplitudes associated with a system of two coupled reactions (TRIS-phenol red) as well as the ternary system (Mg2+-iminodiacetic acid-phenol red) are presented. The termodynamic parameters calculated from experimentally measured temperature perturbation amplitudes using a multiparametric curve fitting procedure are found to be in good agreement with those determined from pH- and costant rate thermometric titrations. For phenol red, pK I =7.55, ΔH I =3.45 kcal, and for Mg2+ iminodiacetic acid, log K M =2.84, ΔH M =3.25 kcal, were obtained. It is shown that this method can be used to determine accurate thermodynamic enthalpy changes over a narrow temperature interval of less than 1.0°C from a single experiment requiring about 50 μl of sample solution.
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  • 19
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    Journal of solution chemistry 12 (1983), S. 771-781 
    ISSN: 1572-8927
    Keywords: Ultrasonics ; kinetics ; aqueous solution ; iso-butyl cellosolve
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Ultrasonic absorption and velocity measurements in aqueous solution of iso-butyl cellosolve (ethylene glycol iso-butyl ether) as a function of the concentration are reported. The two relaxational absorptions have been attributed to the perturbation of the equilibria expressed by AB⇌A+B and Aα(1/n)An where A is the solute, B is the solvent, AB is the complex and A n is the solute aggregate. The rate constants for each step have been determined. From the concentration dependence of the maximum excess absorption per wave length, the enthalpy change and the volume change for the reaction between the solute and the solvent have been determined for aqueous solutions of butyl cellosolve (ethylene glycol n-butyl ether), iso-butyl cellosolve and propyl cellosolve (ethylene glycol n-propyl ether). The results are consistent with a hydrogen bonding reaction. The effect of the ethers on water structure are considered and it is clear that the fraction of water molecules which can hydrogen bond to the solute decreases with the increasing hydrophobicity of the solute.
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  • 20
    ISSN: 1572-8927
    Keywords: Solvolysis ; kinetics ; aqueous solvent mixtures ; Co(III) complexes
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The kinetics of the solvolysis of [Co(CN)5Cl]3− have been investigated in water +2-methoxyethanol and water + diethylene glycol mixtures. Although the addition of these linear hydrophilic cosolvent molecules to water produces curvature in the variation of log(rate constant) with the reciprocal of the dielectric constant, their effect on the enthalpy and entropy of activation is minimal, unlike the effect of hydrophobic cosolvents. The application of a Gibbs energy cycle to the solvolysis in water and in the mixtures using either solvent-sorting or TATB values for the Gibbs energy of transfer of the chloride ion between water and the mixture shows that the relative stability of the emergent solvated Co(III) ion in the transition state compared to that of Co(CN)5Cl3− in the initial state increases with increasing content of cosolvent in the mixture. By comparing the effects of other cosolvents on the solvolysis, this differential increase in the relative stabilities of the two species increases with the degree of hydrophobicity of the cosolvent.
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  • 21
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    Journal of solution chemistry 6 (1977), S. 203-216 
    ISSN: 1572-8927
    Keywords: Glucose ; kinetics ; mixed solvent ; kinetic isotope effect ; enthalpy of activation ; entropy of activation ; tetrahydrofuran ; tert-butanol ; mutarotation
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The mutarotation rates of glucose in aqueous mixtures of tetrahydrofuran andtert-butanol in the mole fraction (xi) range 0〈xi〈0.2 have been measured at 5° intervals in the range 5–35°C. The kinetic deuterium isotope effects have been determined for the same solvent compositions at 25 and 35°C. A statistical analysis of the Arrhenius plots indicates that the experimental errors, although small, are too large for the establishment of any compensation behavior between ΔH
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  • 22
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    Journal of applied electrochemistry 29 (1999), S. 191-200 
    ISSN: 1572-8838
    Keywords: cyclic redox reaction ; dissolution ; kinetics ; manganese dioxide ; mechanism ; pyrite
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Electrical Engineering, Measurement and Control Technology
    Notes: Abstract This paper describes a study of the kinetics and mechanism of MnO2 dissolution in H2SO4 in the presence of pyrite through leaching and electrochemical parameters. Manganese(iv) was found to dissolve mainly through reduction by the ferrous ion generated during oxidation of pyrite by the ferric ion. The oxidation which is slower and rate controlling may proceed through two different reactions, one producing S0 and the other SO42−. Manganese dissolution runs at the same rate as that of pyrite oxidation by maintaining ferrous ion concentration at a much lower level than that of ferric. Kinetic equations based on corrosion coupling principles are developed to explain the observed leaching behaviour.
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  • 23
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    Journal of chemical crystallography 28 (1998), S. 69-72 
    ISSN: 1572-8854
    Keywords: Co(III) complex ; crystal structure ; kinetics ; steric effects
    Source: Springer Online Journal Archives 1860-2000
    Topics: Geosciences , Physics
    Notes: Abstract The title compound crystallizes in the orthorhombic space group Pnma, with a = 7.9209(5), b = 9.818(1), c = 16.867(2) Å, and Z = 4. The structure was solved employing 1864 independent x-ray reflections with I〉2σ(I) by Patterson and difference Fourier techniques and refined by full-matrix least-squares to R = 0.036. The trans-[CO(NH3)4(NH2CH3)Cl](ClO4)2 molecule is on a crystallographic mirror plane. The cobalt ion is in an elongated octahedral coordination with four equatorial ammonia ligands [average Co–N distance equal to 1.966(2) Å], an axial methylamine [Co–N=1.965(3)Å], and an axial chlorine ion [Co–Cl=2.2771(9)Å]. Kinetic steric effects of the complex are interpreted in terms of structural results.
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    Journal of solution chemistry 19 (1990), S. 1073-1084 
    ISSN: 1572-8927
    Keywords: Solvolysis ; kinetics ; mixtures of water+cosolvent
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Rates of solvolysis of the complex cation [Co(4tBupy)4Cl2]+ have been determined in mixtures of water with the hydrophobic solvent, t-butyl alcohol. The solvent composition at which the extremum is found in the variation of the enthalpy ΔH* and the entropy ΔS* of activation correlates well with the extremum in the variation of the relative partial molar volume of t-butyl alcohol in the mixture and the straight line found for the variation of ΔH* with ΔS* is coincident with the same plot for water + 2-propanol mixtures. A free energy cycle is applied to the process initial state (C n+) going to the transition state [M(n+1)+...Cl−] in water and in the mixture using free energies of transfer of the individual ionic species, ΔG t o (i), from water into the mixture. Values for ΔG t o (i) are derived from the solvent sorting method and from the TATB/TPTB method: using data from either method, changes in solvent structure on going from water into the mixture are found to stabilize the cation in the transition state, M(n+1)+, more than in the initial state, C n+. This is compared with the application of the free energy cycle to the solvolysis of complexes [Co(Rpy)4Cl2]+ and [Coen2LCl]+ in mixtures of water with methanol, 2-propanol or t-butyl alcohol: the above conclusion regarding the relative stabilization of the cations holds for all these complexes in their solvolyses in water+alcohol mixtures using values of ΔG t o (Cl−) from either source.
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  • 25
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    Journal of solution chemistry 2 (1973), S. 217-238 
    ISSN: 1572-8927
    Keywords: Cation ; energies ; H. S. Frank ; M. Eigen ; R. G. Wilkins ; kinetics ; ligand substitution ; mechanism ; mixed solvents ; nonaqueous ; solvation ; solvent ; solvent structure ; solvent exchange ; transition metal
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The role of the solvent in reactions involving ions is considered in relation to the structure of liquids. The rate constants and activation parameters for ligand substitutions at divalent transition metal cations in various solvents are compared with those for solvent exchanges. The differences are related to structural properties of the solvents, represented by their heats of evaporation and fluidities, and interpreted with the aid of a model developed from that of Frank and Wen. Water is not a typical solvent.
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  • 26
    ISSN: 1572-8927
    Keywords: Cu(II) ; kinetics ; reduction ; temperature dependence ; H2O2, NaCl, NaBr, NaClO4
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The rates of reduction of Cu(II) with H2O2 have been measured in NaCl and NaBr solutions and mixtures with NaClO4 as a function of pH (6 to 9), temperature (5 to 45°C) and ionic composition (0.1 to 6M). The effect of pH on the rates was found to be independent of temperature and ionic composition. The rates increased as a function of [H+] raised to the power of 1.3 to 1.6. Speciation calculations indicate that this pH dependence can be attributed to Cu(OH)2 being the reactive species. The rate constants in NaCl and NaBr and mixtures with NaClO4 were independent of ionic strength, but proportional to the halide concentration raised to the power of 2.0 (0.2 to 2.6M). These results can be attributed to Cu(OH)2Cl 2 2− being the reactive species to reduction with H2O2. The Cu(I) halide complexes formed from the reduction are not easily oxidized with O2 or H2O2. The faster rates in Br− solutions, which form stronger complexes with Cu+, support this contention. Measurements made in NaCl with added NaHCO3, NaB(OH)4 EDTA, NTA and glycine were also made. These measurements indicate that the CuL complexes (L=B(OH) 4 − , CO 3 2− , EDTA, NTA, and glycine) are not very reactive to reduction with H2O2. The addition of Mg2+ or Ca2+ caused the rates to increase due to the formation of MgL or CaL complexes and the resultant release of reactive Cu2+.
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  • 27
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    Journal of solution chemistry 23 (1994), S. 483-500 
    ISSN: 1572-8927
    Keywords: Thermodynamics ; kinetics ; chemical relaxation ; temperature-jump ; amplitudes
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Amplitudes of chemical relaxation signals can provide useful information as to the thermodynamics of coupled chemical reactions. The temperature-jump technique has been used to investigate the thermodynamic behavior of the Nickel(II)-3,5-dinitrosalicylate system in buffer solution, where complex formation steps are coupled to proton transfer steps. The analysis of the relaxation curves is based on the transformation of a set of coupled elementary reactions into a set of uncoupled ‘normal reactions.’ By analogy with classical titrations, the experiments have been performed by changing the metal ion concentration at constant ligand concentration and pH. Each measured amplitude is associated in this way to a point of a ‘dynamic titration’ and a procedure is formulated by which the values of the equilibrium constants and enthalpies of the normal reactions are simultaneously obtained by simple linear plots. From the dependence of these parameters on suitable functions of the concentrations of the reactants the values of ΔG° and ΔH° of the individual steps are derived. It is shown that the addition of a buffer (instead of an indicator) influences the stoichiometric coefficients of the normal reaction in such a way that measurable amplitudes are produced in systems that, as the presently investigated, in unbuffered solution would remain insensitive to the external perturbation. The circumstances under which the dynamic method offers advantages over the classical techniques are discussed.
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    Journal of solution chemistry 5 (1976), S. 163-169 
    ISSN: 1572-8927
    Keywords: Solvent effects ; tetramethylurea ; hydrolysis ; hydrogen bonding ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Tetramethylurea was hydrolyzed in aqueous hydrochloric acid at temperatures of 80, 90, and 100°C. All reactions were carried out in an excess of both tetramethylurea and water, with first-order dependence on acid concentration being observed. As the concentration of water was increased, the rate of hydrolysis decreased until equimolar amounts of water and tetramethylurea were present. Subsequent addition of water had no effect on the observed rate.
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    Adsorption 1 (1995), S. 133-151 
    ISSN: 1572-8757
    Keywords: PSA process ; sensitivity ; equilibria ; kinetics ; heats
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    Topics: Chemistry and Pharmacology , Physics , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract Mathematical models for pressure swing adsorption (PSA) processes essentially require the simultaneous solutions of mass, heat and momentum balance equations for each step of the process using appropriate boundary conditions for the steps. The key model input variables needed for estimating the separation performance of the process are the multicomponent adsorption equilibria, kinetics and heats of adsorption for the system of interest. A very detailed model of an adiabatic Skarstrom PSA cycle for production of high purity methane from a ethylene-methane bulk mixture is developed to study the sensitivity of the process performance to the input variables. The adsorption equilibria are described by the heterogeneous Toth model which accounts for variations of isosteric heats of adsorption of the components with adsorbate loading. A linear driving force model is used to describe the kinetics. The study shows that small errors in the heats of adsorption of the components can severely alter the overall performance of the process (methane recovery and productivity). The adsorptive mass transfer coefficients of the components also must be known fairly accurately in order to obtain precise separation performance.
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    Adsorption 2 (1996), S. 265-277 
    ISSN: 1572-8757
    Keywords: frequency response ; diffusion cell ; kinetics ; diffusion ; heat effects
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    Topics: Chemistry and Pharmacology , Physics , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract This paper deals with frequency response (FR) analysis of a closed diffusion cell system with two resonators, that is both the LHS and RHS volumes are modulated. The analysis is made for a homogeneous particle described by a single effective diffusivity as well as a biporous pellet described by macropore and micropore diffusions. It is shown that if the perturbation of the volume of the reservoir #2 is lagged behind that of the reservoir #1 by 3π/2, the pressure response in reservoir #1 is significantly enhanced with larger amplitude as well as phase angle. When the perturbations of the two reservoirs are out of phase, the heat effect is reduced and can become insignificant when the two perturbations are completely out of phase (ψ = π). Under such a condition, the pressure difference between the two reservoirs could be doubled. In the case of biporous pellets, it is shown that the FR behaviours obtained for micropore diffusion control and macropore diffusion control are well distinguished. In the former case, the FR system reduces to a traditional batch adsorber one while in the latter case, the FR behaviour is the same as for a two resonator system with homogeneous particles. This difference can be used for the discrimination of micropore and macropore diffusion processes.
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  • 31
    ISSN: 1572-8757
    Keywords: characterisation ; equilibria ; kinetics ; micropore size distribution ; n-butane ; nutshell
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    Topics: Chemistry and Pharmacology , Physics , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract Adsorption equilibria and dynamics ofn-butane on two activated carbon samples prepared from the physical activation of nutshell are studied in this paper. The micropore size distribution (MPSD) is considered as the main source of solid heterogeneity. Lennard-Jones' potential theory and Dubinin's theory (TVFM) are used in the equilibria data to derive the MPSD, which is well fitted by a Gamma distribution function. The adsorption energy distribution derived from the MPSD is very asymmetric for both the samples studied, and this energy distribution used in the HMSD/HMSMD kinetics models for the study of adsorption dynamics ofn-butane.
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  • 32
    ISSN: 1572-8773
    Keywords: acidophilic ; strain ; oxidation ; kinetics
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    Topics: Biology , Chemistry and Pharmacology
    Notes: Abstract Recovery of metal values from sulfide ores by use of acidophilic microorganisms is gaining importance. A number of commercial/pilot plants are setup to find out the techno-economic feasibility of the overall process. The main drawback in the process is the slow kinetics of dissolution of metal values from the sulfide ores. To make the technology e attractive the kinetics should be improved considerably. There are various factors which determine the overall kinetics such as bacterial activity and concentration, iron and sulfur oxidation, oxygen consumption, reactor design and nature of ore. A brief review has been made dealing with the above parameters
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  • 33
    ISSN: 1572-879X
    Keywords: Fischer-Tropsch synthesis ; reaction activation barrier ; carbon chain growth and termination ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract A method is established, by which the difference of the reaction activation barriers of carbon chain growth and termination in Fischer-Tropsch (FT) synthesis can be determined from experiments. A FT synthesis is carried out on Fe/Zn catalyst. We apply the method to analyze the experimental result and obtain the difference of reaction activation barriers of carbon chain growth and termination of α-olefins on the catalyst.
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    Catalysis letters 37 (1996), S. 167-172 
    ISSN: 1572-879X
    Keywords: dissociation ; kinetics ; Co-Mo sulphide ; H2S
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    Topics: Chemistry and Pharmacology
    Notes: Abstract In this study, a high surface area 4Co∶6Mo∶100γ-Al2O3 sulphide prepared using precipitation from homogeneous solution (PFHS) has been used for the catalytic splitting of hydrogen sulphide into H2 and elemental sulphur. The activity of this new formulation was significantly better than previously reported recipes. Kinetic data collected over a wide range of H2S partial pressures between 883 and 983 K revealed that, although the decomposition followed a first-order law, a mechanism involving H2S adsorption on co-ordinative unsaturation sites of the Co-Mo sulphide catalyst gave a Langmuir-Hinshelwood rate expression that yielded satisfactory model parameters. In particular, the scission of the surface H-S bond appeared to be the rate determining step.
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    Cellulose 1 (1994), S. 26-56 
    ISSN: 1572-882X
    Keywords: low-temperature degradation ; kinetics ; mechanisms ; electrical insulation ; transformers
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    Topics: Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract A critical review is given of the degradation of cellulose in the low-temperature region (below about 300°C) of power transformer operation. The large number of kinetic studies, under a variety of environmental conditions from Kraft paper in insulating oil, to cotton and paper in oxygen, are considered in terms of a first-order polymer chain scission model. In many cases, the data are replotted to suit the model. A common activation energy of 111±6 kjmol−1 is calculated and it is shown that the pre-exponential factor, rather than the activation energy, is sensitive to the oxidizing nature of the environment and the susceptibility to degradation of the material. The chemical mechanisms of degradation are reviewed, and conclusions and recommendations are made regarding chemical condition monitoring and life prediction of electrical insulation.
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    Adsorption 6 (2000), S. 137-147 
    ISSN: 1572-8757
    Keywords: adsorption ; kinetics ; linear driving force model ; process design
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    Topics: Chemistry and Pharmacology , Physics , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract The Linear Driving Force (LDF) model for gas adsorption kinetics is frequently and successfully used for analysis of adsorption column dynamic data and for adsorptive process designs because it is simple, analytic, and physically consistent. Yet, there is a substantial difference in the characteristics of isothermal batch uptake curves on adsorbent particles by the LDF and the more rigorous Fickian Diffusion (FD) model. It is demonstrated by using simple model systems that the characteristics of the adsorption kinetics at the single pore or the adsorbent particle level are lost in (a) evaluating overall uptake on a heterogeneous porous solid, (b) calculating breakthrough curves from a packed adsorbent column, and (c) establishing the efficiency of separation by an adsorptive process due to repeated averaging of the base kinetic property. That is why the LDF model works in practice.
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    Catalysis letters 37 (1996), S. 173-179 
    ISSN: 1572-879X
    Keywords: ammonia synthesis ; iron catalysts ; potassium promotion ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Measurements were performed of reaction rate in the process of ammonia synthesis (T=370–470°C) on doubly promoted (DP) (Al2O3, CaO) and triply promoted (TP) (K2O, Al2O3, CaO) iron catalysts. The latter were obtained by impregnation of the reduced and subsequently passivated DP precursors with alcoholic solution of KOH. The studies were carried out under high total pressure (10 MPa) in a wide range of ammonia partial pressure in the gas phase: from 0.25 to about 7 bar. The results are shown to be authoritative for the so-called kinetic regime. The effect of the presence of K+ cations in the catalyst was the stronger, as the temperature of the reaction was the lower and, in particular, the ammonia pressure in the gas phase the higher. The obtained results are in good accordance with the results of Somorjai's studies on activity of iron single crystal surfaces both clean and covered with (K+O) adlayer.
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    Catalysis letters 27 (1994), S. 79-90 
    ISSN: 1572-879X
    Keywords: kinetics ; carbon ; oxygen ; recombination ; rhodium ; surface characterisation ; XPS ; AES
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Different mechanisms of atomic carbon and oxygen recombination on a rhodium surface are studied with Auger electron spectroscopy (AES) and X-ray photoelectron spectroscopy (XPS). The kinetics of adsorbed carbidic carbon oxidation (carbon coverageθ c ≈ 0.1–0.3 ML) by gas-phase oxygen that proceeds by a Langmuir-Hinshelwood reaction mechanism, provides the value of the activation energy for recombination (E rec ⇂t ≈ 170±20 kJ/mol).E rec ⇂t depends slightly on the carbon coverage. An Eley-Rideal type of reaction was observed for adsorbed oxygen and atomic gas-phase carbon recombination which occurs in a dynamic regime. The low value found for the activation energy (near zero) is consistent with the mechanism that this exothermic reaction is too fast for energy dissipation into the substrate; the energy is mainly transferred into translational, vibrational and rotational energy of CO.
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  • 39
    ISSN: 1572-879X
    Keywords: ammonia synthesis ; kinetics ; ruthenium catalysts ; promotional effect
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The kinetics of NH3 synthesis over carbon-based ruthenium catalysts promoted with barium or alkali was studied. Both the ammonia partial pressure dependencies of the reaction rates (T = 400°C, p = 63 bar, H2 : N2 = 3 : 1) and the pressure variations of the activity (T = 370°C, p= 4–63 bar, H2 : NN2 = 3 : 1) were found to be different for Ba and for the alkali (K, Cs). Ba–Ru/C proved to be more sensitive to the NH3 content and to the total pressure. The rate of synthesis over the alkali-promoted catalysts is, in turn, much stronger influenced by the ruthenium dispersion. TOFs of NH3 synthesis for the promoted samples at 370°C and 4 bar (Ba 0.085 1/s, Cs 0.05 1/s, K 0.035 1/s) are significantly higher than that for the Ru(0001) basal plane (0.0085 1/s results from the literature data at 370°C, 2 bar). The most active Ru/C samples (Ba or Cs) exceed significantly the fused iron catalyst, especially at high conversions.
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  • 40
    ISSN: 1572-882X
    Keywords: accelerated tests ; aging tests ; cellulose degradation ; durability ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract Accelerated aging tests are credible and useful to predict paper permanence only if such tests can be shown to correlate with natural aging. In the first part of this study, a kinetic model was developed based on the accelerated aging results. In this report, we have shown that this kinetic model can indeed predict the natural aging results of lignin-free sheets with a statistical confidence. This is the first quantitative comparison of accelerated aging with natural aging.
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    Journal of solution chemistry 27 (1998), S. 1123-1138 
    ISSN: 1572-8927
    Keywords: Sol–gel processing ; hydrolysis ; condensation ; kinetics ; methoxydimethyloctylsilane ; copper nitrate hydrate ; phase diagram
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The reaction rate was determined for copper nitrate hydrate with methoxydimethyloctylsilane (MDOS) in methanol. The rate constants of hydrolysis and condensation were established by quantitative measurement of the product and Karl Fischer water determination. The reaction with the hydrated copper salt resulted in the phase separation of an insoluble product from the reaction mixture. The structure of the product was determined, by Fourier Transform Infrared Spectrometry (FTIR) and Nuclear Magnetic Resonance (NMR) to be a dimer of the MDOS. The results showed the alcohol, producing condensation reaction was negligible in the formation of the dimer. contrary to the case for the well-known reaction by trialkoxysilanes and tetraalkoxysilanes.
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  • 42
    ISSN: 1572-8927
    Keywords: Enthalpies of reaction ; heats of reaction ; kinetics ; ester hydrolysis ; microcalorimetry
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The conditions under which the Picker flow microcalorimeter can be used to measure enthalpies and rates of reactions were investigated. For this purpose, systematic studies were made of the enthalpies of neutralization of HCl, HBr, HNO 3 , acetic, proprionic, and butyric acids with NaOH, enthalpies of hydrolysis of methyl and ethyl acetate with NaOH, and the reaction rates of the ester hydrolysis with NaOH. The general procedure and various sources of error are discussed and it is concluded that enthalpies of slow reactions can be measured to about 1% when the calorimeter is operated in the quasi-isothermal mode and the reaction rates to about 3% when operated in the quasi-adiabatic mode.
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    Cellulose 4 (1997), S. 1-5 
    ISSN: 1572-882X
    Keywords: paper ; degradation ; ageing ; kinetics ; modelling
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    Topics: Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition , Process Engineering, Biotechnology, Nutrition Technology
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    Cellulose 3 (1996), S. 243-267 
    ISSN: 1572-882X
    Keywords: aging tests ; cellulose degradation ; durability ; kinetics ; paper properties
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    Topics: Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract The validity of accelerated aging tests to predict and rank papers on their permanence has been under question, preventing the development of performance-based standards for permanent paper. We conducted a general kinetic analysis to investigate the aging process of paper. A general kinetic model is proposed to describe the depolymerization of cellulose. Experimentally it was shown that in the case of aging, cellulose degradation follows classic first-order kinetics as a special case of our general kinetic model. The Arrhenius equation was critically re-examined for the case of a multiple reaction system. It was shown analytically that the Arrhenius equation is still applicable when certain conditions are met. This was convincingly supported by experimental results. We also analysed the dependence of the degradation rate on the moisture content and hydrogen ion concentration. By conducting systematic experiments on these two factors, a general and quantitative relationship was established to explain the contribution of each factor and their interactions. Finally, based on this kinetic analysis, the effects of storage conditions on the life expectancy of paper were estimated.
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    Journal of solution chemistry 3 (1974), S. 881-887 
    ISSN: 1572-8927
    Keywords: Binary aqueous mixtures ; solubilities ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract A treatment which predicts the solubilities of gases in solvent mixtures is examined in the context of the analysis of kinetic data for reactions in aqueous mixtures. The treatment is qualitatively successful to some extent in resolving the effects of changes in the initial state of the reacting substrate in the activation parameters.
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    Journal of inorganic and organometallic polymers and materials 8 (1998), S. 111-117 
    ISSN: 1572-8870
    Keywords: Organosiloxane ; kinetics ; poly(phenylmethylsiloxane) ; catalyst ; anionic ; ring-opening
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    Topics: Chemistry and Pharmacology
    Notes: Abstract It is well known that the rate of polymerization for an anionic mechanism is dependent on the ability of the bulk material or solvent system to disassociate the ion pair at the propagating chain end. In the anionic ring-opening polymerization of cyclic organosiloxanes in particular, the larger and softer the counter ion, the more rapidly the reaction proceeds. A recently developed phosphazene initiator system provides a large, soft counter ion relative to other traditional initiators used for the polymerization of poly(dimethylsiloxane) (PDMS). This novel initiator system was used in this investigation for the ring-opening polymerization of tetraphenyltetramethylcyclotetrasiloxane (P4) and the reaction kinetics under bulk and solution conditions were investigated. The new initiator system showed a dramatic increase in the rate of polymerization over the conventional potassium hydroxide-catalyzed system. Furthermore, this initiator was sufficiently reactive to be useful for the ring-opening polymerization of P4 at 293 K.
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  • 47
    ISSN: 1572-8900
    Keywords: Cellulose ; alkaline degradation ; peeling off ; degree of polymerization ; kinetics ; (gluco)isosaccharinic acid
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Energy, Environment Protection, Nuclear Power Engineering , Mechanical Engineering, Materials Science, Production Engineering, Mining and Metallurgy, Traffic Engineering, Precision Mechanics
    Notes: Abstract The degradation of cellulosic materials, differing mainly in the degree of polymerization and the number of reducing end groups, was studied under the alkaline conditions similar to those existing in a cementitious repository for low- and intermediate-level radioactive waste (pH 13.3, T = 25°C). The kinetics of alkaline degradation (peeling-off reaction) were studied and the data analyzed by the model of Haas et al. [13]. The observed kinetic parameters for the propagation reaction and overall stopping reaction were compared with literature data. Although measured under different experimental conditions, literature data and data from this study show a consistent picture. Differences in the extent of degradation observed for the different cellulosic materials could be satisfactorily explained by differences in reducing end group content and, consequently, by differences in the degrees of polymerization. Besides the number of reducing end groups, the degree of amorphousness also plays an important role. The main degradation products formed under the experimental conditions used are α- and β-(gluco)isosaccharinic acid. This is in agreement with many other studies on alkaline degradation of cellulose. The two isomers are formed in roughly equal amounts.
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    Journal of solution chemistry 15 (1986), S. 221-229 
    ISSN: 1572-8927
    Keywords: Ultrasonics ; kinetics ; aqueous solution ; triethylene glycol monobutyl ether
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The ultrasonic absorption from 6.5 to 220 MHz and velocities at 2.5 MHz have been measured in aqueous solution of triethylene glycol monobutyl ether as a function of concentration at 25°C. A single relaxational excess absorption, observed from 0.60 to 2.5 mol-dm−3, is attributed to a perturbation of an equilibrium associated with solute-solvent interaction. Rate constants for the forward and reverse processes have been determined from the concentration dependence of the relaxation frequency, and the influence on the water structure by an addition of the solute has been considered. Solution densities were also measured in order to obtain the expansivity of the solution. The standard volume and enthalpy changes of the reaction have been estimated from the concentration dependence of the maximum excess absorption per wave length. A linear relationship between the number of oxyethylene groups and the free energy change between bonded water and nonbonded water is established.
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    Topics in catalysis 5 (1998), S. 133-147 
    ISSN: 1572-9028
    Keywords: NMR ; catalysis ; high pressure ; dynamic equilibria ; magnetization transfer ; sapphire tube ; gas phase ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract High resolution NMR techniques are applicable to a variety of aspects of catalysis. Methods for studying homogeneously-catalyzed systems under high gas pressure are described along with approaches for obtaining mechanistic and dynamic information. Many of the same techniques may be applied to heterogeneous catalysis by following the reaction chemistry by gas phase NMR.
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  • 50
    ISSN: 1572-9028
    Keywords: nonlinear temperature behavior ; Eyring plot ; modified Eyring plot ; selectivity ; selection process ; enantioselectivity ; selection level ; isoinversion principle ; isoinversion temperature ; inversion temperature ; kinetics ; catalysis ; asymmetric hydrogenation ; dihydroxylation ; cocyclization
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The influence of the temperature on selectivity is described under special consideration of nonlinearities in the corresponding modified Eyring plots. Reasons for the experimentally well-known behavior are discussed. Furthermore, the conditions for nonlinear temperature behavior are quantified and a concept is described which allows the determination of the temperature dependence of a single reaction pathway in a selection process.
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    Topics in catalysis 1 (1994), S. 305-314 
    ISSN: 1572-9028
    Keywords: non-Langmuir ; kinetics ; non-linear dynamics ; oscillations ; chaos ; self-organization
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The kinetics of a catalytic reaction is frequently formulated in terms of simple concepts of the Langmuir type. Apart from limitations arising from the non-uniformity of the catalyst's surface and from the coverage dependence of the rate “constants”, several other complications may come into play. These may arise on the “quantum level” where energy flow between the various degrees of freedom may cause failure of simple transition state theory, as well as on the “continuum level” where formulation of rate equations in terms of coupled non-linear differential equations may give rise to a rich scenario of spatio-temporal self-organization, including kinetic oscillations, chaos, and formation of concentration patterns. Several of these phenomena are illustrated by selected examples.
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  • 52
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    Topics in catalysis 11-12 (2000), S. 327-333 
    ISSN: 1572-9028
    Keywords: hydrodenitrogenation ; toluidine ; methylcyclohexylamine ; kinetics ; nickel-promoted molybdenum sulphide
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The hydrodenitrogenation (HDN) of o-toluidine and its reaction intermediates was studied over a NiMo/γ-Al2O3 catalyst. The kinetics of the HDN of methylcyclohexylamine and of the hydrogenation of cyclohexene were also studied. Hydrogenation of o-toluidine alone produces methylcyclohexene and methylcyclohexane. When a sufficient quantity of cyclohexene is added during the HDN of toluidine, methylcyclohexylamine, the first intermediate in the hydrogenation of toluidine, becomes detectable. Because of its strong adsorption constant and high rate constant for reacting further to methylcyclohexene and methylcyclohexane, methylcyclohexylamine is not observed in the HDN of toluidine. Adding cyclohexene decreases the adsorption of methylcyclohexylamine, thus enabling its detection. The rate and adsorption constants of methylcyclohexylamine and cyclohexene in the HDN of methylcyclohexylamine were calculated by fitting the kinetic data to a Langmuir–Hinshelwood equation. A two-site model was used to describe the surface reactions, with one site for the methylcyclohexylamine reactions and the other for the cyclohexene reaction.
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  • 53
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    Cellular and molecular life sciences 49 (1993), S. 110-117 
    ISSN: 1420-9071
    Keywords: Polymerization ; sickle hemoglobin ; sickle cell disease ; kinetics ; thermodynamics ; polymer domains ; nucleation
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Medicine
    Notes: Abstract The polymerization of sickle hemoglobin occurs by the same mechanisms in solutions and in cells, and involves the formation of 14 stranded fibers from hemoglobin molecules which have assumed a deoxy quaternary structure. The fibers form via two types of highly concentration-dependent nucleation processes: homogeneous nucleation in solutions with hemoglobin activity above a critical activity, and heterogeneous nucleation in similarly supersaturated solutions which also contain hemoglobin polymers. The latter pathway is dominant, and creates polymer arrays called domains. The individual polymers bend, but also cross-link, and the resulting mass behaves as a solid. The concentration of polymerized hemoglobin increases exponentially unless clamped by rate limiting effects such as oxygen delivery.
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  • 54
    ISSN: 1438-1168
    Keywords: Scandium ; tin ; beryllium ; mineralogy ; geochemistry ; pegmatite ; Scandium ; Zinn ; Beryllium ; Mineralogie ; Geochemie ; Pegmatit
    Source: Springer Online Journal Archives 1860-2000
    Topics: Geosciences
    Description / Table of Contents: Zusammenfassung In Tørdal durchschneiden Granit-pegmatitische Gänge eine vulkano-sedimentäre Abfolge, die über einem älteren Gneis-Basement und einem jüngeren Granit, von dem die Gänge stammen, liegt. Positive Kovariation von Scandium, Lithium, Beryllium und Zinn, die sich im Zuge eines Prospektionsprogrammes auf Zinn ergaben, deuten auf eine mögliche Anreicherung von Scandium und Zinn während des Aufstieges pegmatitischer Phasen durch die vulkano-sedimentäre Abfolge hin. Ein Scandium-reicher Ixiolit in Assoziation mit Pyrochlor und Bazzit wird beschrieben, der aus einem Clea-velandit-Amazonit-Pegmatit stammt. Der Pegmatit bildet einen Teil eines größeren Netzwerkes von granit-pegmatischen Gängen. Eine Alteration von Ixiolit zu Pyrochlor tritt als spätmagmatisch-hydrothermales Ereignis auf.
    Notes: Summary In Tørdal granite pegmatite veins cut through a volcano-sedimentary sequence which overlies an older, gneissic basement and younger granite from which they originate. Positive co-variations of scandium, lithium, beryllium and tin, which were documented through a recent prospecting program for tin, indicate a possible enrichment of scandium and tin during the passage of the pegmatitic material through the volcanic sedimentary sequence. A description is given of scandium-rich ixiolite, (Ta,Nb,Sc,Sn,Fe,Mn,Ti)2O4 in association with pyrochlore, (Ca,Sc,Y,Sn,U)2(Ta,Nb,Ti)2O6(O,OH,F) and bazzite, Be3Sc2Si6O18 from a cleavelandite-amazonite pegmatite occurring as a part of a larger network of granitic pegmatite veins. Alteration from ixiolite to pyrochlore appears as a late magmatic-hydrothermal event.
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  • 55
    ISSN: 1572-8757
    Keywords: micropore size distribution ; activated carbon ; adsorption ; desorption ; equilibrium ; kinetics
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    Topics: Chemistry and Pharmacology , Physics , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract This paper deals with the prediction of adsorption equilibrium and kinetics of hydrocarbons onto activated carbon samples having different micropore size distribution (MPSD). The microporous structure of activated carbon is characterised by the distribution of slit-shaped micropores, which is assumed to be the sole source of surface heterogeneity. The interaction between adsorbate molecule and pore walls is described by the Lennard-Jones potential theory. Different adsorbates have access to different pore size range of activated carbon due to the size exclusion, a phenomenon could have a significant influence on both multicomponent equilibria and kinetics. Activated carbons with three different MPSDs are studied with ethane and propane as the two model adsorbates. The Heterogeneous Macropore Surface Diffusion model (HMSD) is employed to simulate adsorption kinetics. The simulation results show that the MPSD is an important factor affecting both the multicomponent equilibria and kinetics.
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  • 56
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    Adsorption 6 (2000), S. 349-357 
    ISSN: 1572-8757
    Keywords: sulfadiazene ; adsorption ; kinetics
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    Topics: Chemistry and Pharmacology , Physics , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract To investigate the nature of interactive forces between sulfadiazene molecules and alumina surface the experiments were performed for the adsorption of sulfadiazene (SD) from its aqueous sulution onto the alumina surfaces at 25 ± 0.2°C and the influence of factors such as increasing concentration of SD (4.0–20.0 × 10−3 mol cm−3), the time required for adsorption equilibrium, pH (2.0–12.0) and temperature (5–45°C) of the adsorption medium, the presence of ions like Cl−, SO2− 4 and PO3− 4 (0.01–0.30 M) and organic solvents (5% v/v) were observed on the course of adsorption of SD. Various adsorption and kinetic parameters such as adsorption coefficient, the rate constants for adsorption and desorption were also evaluated. The results of the above cited studies facilitated to formulate the mechanisms of interaction between SD and alumina surfaces. From application view point the present work may be a potential tool for an effective chromatographic separation of sulfa drugs from industrial effluents.
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  • 57
    ISSN: 1572-879X
    Keywords: propane ; oxidation ; platinum ; palladium ; sulfur dioxide ; alumina ; zirconia ; activity ; acidity ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Earlier studies have shown that sulfur dioxide and metal-support interaction can strongly influence propane oxidation over platinum. In particular, oxidation activity is enhanced when platinum is supported on sulfated γ-alumina or zirconia compared to γ-alumina. Therefore, it is of interest to compare the performance of palladium under the same experimental conditions. Four model catalysts were examined: Pt/γ-alumina, Pt/zirconia, Pd/γ-alumina and Pd/zirconia. The metal loading was kept at or below 0.05 wt% to emphasize changes in activity attributable to metal-support interaction. Reaction rates were measured with and without sulfur dioxide. Surface sulfation was analyzed by measuring acid strength and evaluating spectra obtained by Fourier-transform infrared spectroscopy. In contrast to platinum, sulfation does not promote propane oxidation on Pd/γ-alumina, and Pd/zirconia is less active than Pd/γ-alumina.
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  • 58
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    Catalysis letters 60 (1999), S. 51-57 
    ISSN: 1572-879X
    Keywords: furfural hydrogenation ; Cu/carbon catalysts ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Furfural hydrogenation over copper dispersed on three forms of carbon – activated carbon, diamond and graphitized fibers – were studied. Only hydrogenation of the C=O bond to form either furfuryl alcohol or 2‐methyl furan occurred at temperatures from 473 to 573 K. Reduction at 573 K gave the most active catalysts, all three catalysts had activation energies of 16 kcal/mol, and turnover frequencies were 0.018–0.032 s-1 based on the number of Cu0 + Cu+ sites, which were counted by N2O adsorption at 363 K and CO adsorption at 300 K, respectively. The Cu/activated carbon catalyst showed no deactivation during 10 h on stream, in contrast to the other two catalysts. A simple Langmuir–Hinshelwood model invoking two types of sites was able to fit all kinetic data quite satisfactorily, thus it was consistent with the presence of both Cu0 and Cu+ sites.
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  • 59
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    Catalysis letters 60 (1999), S. 167-171 
    ISSN: 1572-879X
    Keywords: ammonia decomposition ; iron catalyst ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The decomposition of ammonia is a reaction associated with the process of the nitriding of metals. The kinetics of the ammonia decomposition on iron catalysts has been studied using a differential reactor with internal mixing. The balance between the inlet and outlet ammonia quantity has been used to determine the degree of conversion. The rate of ammonia decomposition could be described by the following expression: r = k0 exp (Ea/RT)pNH3. The activation energy of the ammonia decomposition process has been found for samples with potassium as E a= 96 kJ/mol, for samples without potassium as E a= 87 kJ/mol.
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  • 60
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    Catalysis letters 64 (2000), S. 65-75 
    ISSN: 1572-879X
    Keywords: NO reduction ; CH3OH ; La2O3 ; methyl nitrite ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Nitric oxide (NO) reduction by methanol was studied over La2O3 in the presence and absence of oxygen. In the absence of O2, CH3OH reduced NO to both N2O and N2, with selectivity to dinitrogen formation decreasing from around 85% at 623 K to 50–70% at 723 K. With 1% O2 in the feed, rates were 4–8 times higher, but the selectivity to N2 dropped from 50% at 623 K to 10% at 723 K. The specific activities with La2O3 for this reaction were higher than those for other reductants; for example, at 773 K with hydrogen a specific activity of 35 μmol NO/s m2 was obtained whereas that for methanol was 600 μmol NO/s m2. The Arrhenius plots were linear under differential reaction conditions, and the apparent activation energy was consistently near 14 kcal/mol with CH3OH. Linear partial pressure dependencies based on a power rate law were obtained and showed a near‐zero order in CH3OH and a near‐first order in H2. In the absence of O2, a Langmuir–Hinshelwood type model assuming a surface reaction between adsorbed CH3OH and adsorbed NO as the slow step satisfactorily fitted the data, and the model invoking two types of sites provided the best fit and gave thermodynamically consistent rate constants. In the presence of O2 a homogeneous gas‐phase reaction between O2, NO, and CH3OH occurred to yield methyl nitrite. This reaction converted more than 30% of the methanol at 300 K and continued to occur up to temperatures where methanol was fully oxidized. Quantitative kinetic studies of the heterogeneous reaction with O2 present were significantly complicated by this homogeneous reaction.
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  • 61
    ISSN: 1572-8757
    Keywords: kinetics ; isotope-exchange ; nitrogen ; adsorption ; methane ; zeolite ; equilibria
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology , Physics , Process Engineering, Biotechnology, Nutrition Technology
    Notes: Abstract The Isotope Exchange Technique (IET) was used to simultaneously measure pure and binary gas adsorption equilibria and kinetics (self-diffusivities) of CH4 and N2 on pelletized 4A zeolite. The experiment was carried out isothermally without disturbing the adsorbed phase. CH4 was selectively adsorbed over N2 by the zeolite because of its higher polarizability. The multi-site Langmuir model described the pure gas and binary adsorption equilibria fairly well at three different temperatures. The selectivity of adsorption of CH4 over N2 increased with increasing pressure at constant gas phase composition and temperature. This curious behavior was caused by the differences in the sizes of the adsorbates. The diffusion of CH4 and N2 into the zeolite was an activated process and the Fickian diffusion model described the uptake of both pure gases and their mixtures. The self-diffusivity of N2 was an order of magnitude larger than that for CH4. The pure gas self-diffusivities for both components were constants over a large range of surface coverages (0 〈 θ 〈 0.5). The self-diffusivities of CH4 and N2 from their binary mixtures were not affected by the presence of each other, compared to their pure gas self-diffusivities at identical surface coverages.
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  • 62
    ISSN: 1572-8773
    Keywords: aromatic donor molecules ; horseradish peroxidase ; kinetics ; lactoperoxidase
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    Topics: Biology , Chemistry and Pharmacology
    Notes: Abstract Based on kinetic evidence, it has been shown for the first time that the mode of binding of aromatic donor molecules is similar in horseradish peroxidase and lactoperoxidase; also that the nature of the heme plays an important role in the reaction with hydrogen peroxide, and has no effect on the reaction of the intermediate compound II with aromatic substrates.
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  • 63
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    Catalysis letters 31 (1995), S. 431-438 
    ISSN: 1572-879X
    Keywords: partial hydrogenation of benzene ; production of cyclohexene ; kinetics ; reaction mechanism ; ruthenium catalyst
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    Topics: Chemistry and Pharmacology
    Notes: Abstract A method has been developed for direct measurement of reaction rates in a continuously operated slurry (CST-) reactor. In contrast to the usual procedure in a two-liquid-phase system the reactor contains only one liquid phase, an aqueous zinc chloride solution in which a ruthenium lanthanoxide catalyst is suspended. The selectivity of benzene hydrogenation with respect to cyclohexene is higher when the new one-liquid-phase procedure is applied. With decreasing degree of benzene conversion the selectivity with respect to cyclohexene approaches 100%. The conclusion is that cyclohexane is formed only by consecutive hydrogenation of cyclohexene.
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  • 64
    ISSN: 1572-879X
    Keywords: non-uniform surface ; kinetics ; ethanol ; oxidation ; molybdenum oxide
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract Temkin's theory of rates of catalytic reactions on non-uniform surfaces is extended to the MoO3-catalyzed oxidation of ethanol to acetaldehyde. Two types of sites are assumed to be present, an oxygen atom site that can be modeled with uniform properties and a metal atom site characterized by non-uniform properties both for ethanol chemisorption to an ethoxide intermediate and the conversion of this intermediate to acetaldehyde. The rate-limiting step is the cleavage of a C-H bond in the absorbed ethoxide intermediate. Non-uniform surface kinetics leads to a kinetic rate expression of the form $$v = kP_{C_2 H_5 OH}^{1 - m} P_{O_2 }^{(1 - m)/4} P_{H_2 O}^{ - (1 - m)/2} $$ . Such a rate expression, withm=0.14, is shown to provide a good fit to kinetic data for the selective oxidation of ethanol on a silica supported molybdenum oxide catalyst.
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  • 65
    ISSN: 1572-879X
    Keywords: Ultraviolet heterogeneous photocatalysis ; oxidation ; trichloroethylene ; titania ; kinetics
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Kinetics of the gas/solid heterogeneous photocatalytic oxidation of dilute trichloroethylene (TCE) vapors by ultraviolet-illuminated titanium dioxide have been determined using a fixed-bed dynamic photoreactor. Reaction rate dependences on inlet TCE, oxygen and water vapor concentrations were found to consist of both reactant sensitive and insensitive regions. In the reactant sensitive regions, measured limiting apparent reaction rate orders for TCE, oxygen and water vapor are 0.8, 1.7 and — 3, respectively. Water vapor in the reactant stream lowersinitial reaction rates relative to corresponding water free conditions, but is required to sustain photocatalytic activity for extended periods of time.
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  • 66
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    Catalysis letters 36 (1996), S. 31-36 
    ISSN: 1572-879X
    Keywords: ethanol ; kinetics ; oxidation ; oxydehydrogenation ; platinum ; structure sensitivity
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The effect of the platinum particle size was investigated for the catalytic oxidative dehydrogenation of aqueous ethanol to ethanal at a temperature of 303 K, an ethanol concentration of 260 mol m−3, a partial oxygen pressure 60 kPa, a pH of 9, and an ethanal and ethanoate concentration of 20 mol m−3. A particle size effect on the turnover frequency was observed but only for particle sizes smaller than 2 nm. Hence, the reaction shows a limited structure sensitivity.
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  • 67
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    Catalysis letters 55 (1998), S. 73-77 
    ISSN: 1572-879X
    Keywords: enantioselectivity ; hydrogenation of ethyl pyruvate ; Pt/alumina catalyst ; solvent effects ; kinetics ; solvent polarity
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The influence of solvent on the kinetics of enantioselective hydrogenation of ethyl pyruvate by Pt/Al2O3/dihydrocinchonidine is reported. In a non‐polar solvent, toluene, the reaction is approximately zero order in substrate at constant hydrogen pressure, while under the same conditions and at the same substrate concentration, in the polar solvents ethanol and propylene carbonate the reaction shows a first‐order substrate concentration dependence. Fits to a Michaelis–Menten rate expression show that these differences are the expression of the relative magnitudes of the adsorption term in the rate expression, which in turn reflects the influence of the solvent on the adsorption–desorption processes which take place at the catalyst surface.
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  • 68
    ISSN: 1572-879X
    Keywords: hydrogen ; desorption ; copper ; activation energy ; kinetics ; order of desorption
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The kinetics of desorption of hydrogen from the copper component of an alumina-supported polycrystalline copper catalyst has been studied in detail by temperature-programmed desorption (TPD). Line-shape analysis of the hydrogen TPD spectra shows: (i) that the desorption is second order, (ii) that the desorption activation energy is in the range 64–68 kJ mol−1 in the coverage range 7–44% of a monolayer, and (iii) that the desorption pre-exponential term has a value ∼10−5 cm2 s−1 atom−1 consistent with the desorption being second order, involving mobile adsorbates and a mobile desorption transition state.
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  • 69
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    Catalysis letters 69 (2000), S. 103-107 
    ISSN: 1572-879X
    Keywords: dicyclopentadiene ; Wacker oxidation ; Pd(AcO)2 ; benzoquinone ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Chemistry and Pharmacology
    Notes: Abstract The oxidation of dicyclopentadiene catalyzed by palladium(II) acetate and benzoquinone in the presence of perchloric acid was studied. Tricyclodecenone in high selectivity (85–98%) at a conversion of dicyclopentadiene up to 76% was obtained. The kinetic model assumed the significant inhibition complexation between dicyclopentadiene and tricyclodecenone with the catalytic species.
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  • 70
    ISSN: 1432-0819
    Keywords: Arc volcano ; magma mixing ; geochemistry ; alkaline ; calc-alkaline ; sector collapse
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    Topics: Geosciences
    Notes: Abstract The Platanar volcanic center is dominated by a calc-alkaline, basalt-andesite-dacite-rhyolite magma series with unusual LREE enrichment. Adjacent and overlapping the calc-alkaline rocks are the most alkaline basalts found along the volcanic front of Central America. These basalts are mafic, LIL- and LREE-enriched transitional to alkaline basalts. Several are found on the north flank of Platanar in the Aguas Zarcas region, where there are nine cinder cones and a few isolated flows. However, they are also found in isolated lava outcrops at least as far south as Porvenir volcano along the volcanic front. The addition of mafic alkaline magmas with high La/Yb and low Ba/La into the Platanar magma chamber or chambers may contribute to the LREE-enriched character of the Platanar basaltic andesites and andesites. At Platanar the field and geochemical evidence suggest mixing between calc-alkaline and alkaline magmas, a process that has probably occurred throughout the development of the Cordillera Central of Costa Rica. The presence of negative Ce anomalies in several of the calc-alkaline lavas also make the Platanar complex very unusual compared to the rest of the Central American volcanic front. In the center of the Platanar complex is the Chocosuela caldera, an apparent remnant of an avalanche caldera created by the collapse in the Middle Pleistocene of an ancestral stratovolcano toward the NNW in a directed blast-type eruption. Rhyolite is present as pumice lapilli in pyroclastic flow deposits outside the caldera rim. Whole lapilli analyses span the daciterhyolite range. The previous eruption of high silica tephra as pyroclastic flows, the current long dormant period and the repeated occurrence of earthquake swarms on the flanks of the Platanar complex make it a candidate for volcanic hazard mapping, detailed geological mapping and emergency planning.
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  • 71
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    Microchimica acta 94 (1988), S. 277-278 
    ISSN: 1436-5073
    Keywords: kinetics ; FT-IR ; temporal resolution
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    Topics: Chemistry and Pharmacology
    Notes: Abstract A system for performing gas-phase rapid scanning Fourier transform infrared time-resolved Spectrometry (FT-IR/TRS) has been evaluated. This technique can be applied to the study of the lifetimes and reactivity of transient species and can provide detailed information regarding reaction rate constants. Temperature-jump experiments have been initiated and preliminary results are presented.
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    Microchimica acta 94 (1988), S. 323-328 
    ISSN: 1436-5073
    Keywords: FTIR spectroscopy ; kinetics ; polymers ; rheo-optics ; variable-temperature measurements
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The rapid-scanning capability of FTIR instrumentation has revitalized the field of vibrational spectroscopy in polymer research and will be discussed with reference to the study of polyurethane kinetics, the temperature dependence of hydrogen bonding in polyamide 6 and strain-induced crystallization in a polydimethylsiloxane elastomer.
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  • 73
    ISSN: 1436-5073
    Keywords: flow injection analysis (FIA) ; mercury ; porphyrin ; kinetics ; spectro-photometry
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    Topics: Chemistry and Pharmacology
    Notes: Abstract 5,10,15,20-tetrakis(3-chloro-4-sulfophenyl)porphine (m-Cl-TPPS4) was synthesized and used for the Spectrophotometric determination of mercury by flow injection analysis. A pseudo-first-order reaction kinetic mechanism was proposed with a rate constant of 0.8 min−1 for Hg(II) withm-Cl-TPPS4 in the presence of 8-hydroxyquinoline in a medium of 1.0M acetic acid and sodium acetate buffer solution (pH 6.22). In the optimum conditions of reaction temperature (85 ° C), stopped-flow time (60 s) and sampling volume (100 μl), the method's relative standard deviation was 0.82% (n = 12) at 5.0 μg ml−1 mercury, with a linear range of 0–12.0 μg ml−1 and an analytical frequency of 60h−1. The detection limit (3σ) was 0.025 μg ml−1. Interference studies showed that most metal ions co-existing with Hg2+ could be tolerated at 100-fold excess levels, but Zn2+, Cu2+ and Mn2+ needed to be masked. The method has been applied to the analysis of water samples with satisfactory results.
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  • 74
    ISSN: 1436-5073
    Keywords: atrazine ; terbuthylazine ; sequential binding ; kinetics ; cross-reactivity
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    Topics: Chemistry and Pharmacology
    Notes: Abstract Immunoassays for triazine herbicides were tested for their reaction to the variation of the tracer incubation time. By application of a sequential technique the measuring range of atrazine could be expanded to five decades and the total duration of the test could be reduced to about 30 min. In an optimized version a lower detection limit of 9 pmol/l (2 ng/l) was achieved. The detection limit of a sensitive immunoassay for terbuthylazine is also below the concentration limit demanded of the German drinking water regulation (100 ng/l) and reaches 130 pmol/l (30 ng/l). Short tracer incubation times did not lead to increased cross-reactivities in contrast to theoretical models [1, 2]. Different mechanisms, which could cause a shift of the center point of the calibration curve, are discussed, including kinetic considerations.
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  • 75
    ISSN: 1436-5073
    Keywords: kinetics ; rates ; integrating ratemeter ; optimization ; first-order
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    Topics: Chemistry and Pharmacology
    Notes: Abstract The integrating ratemeter is used in concert with the two-rate parameter to form the integrating ratemeter two-rate parameter. Propagation of error theory is applied to the integrating ratemeter two-rate parameter to yield expressions for the precision of rates calculated from the integrating ratemeter two-rate parameter in terms of the precision of the rates measured with the integrating ratemeter. Simulations and experimental results show that in cases where the standard deviation of the rate is relatively constant, the optimum time to make a rate measurement using the integrating ratemeter is also the optimum time to measure either of the rates in the two-rate parameter. If either of the two rates comprising the two-rate parameter is measured at the optimum time, then the precision and accuracy of concentrations measured with this technique are optimized.
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  • 76
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    Biodegradation 4 (1993), S. 163-170 
    ISSN: 1572-9729
    Keywords: factorial analysis ; kinetics ; methane ; methanotrophs ; nutrients
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Energy, Environment Protection, Nuclear Power Engineering , Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition
    Notes: Abstract The effect of different mineral nutrients on the kinetics of methane biodegradation by a mixed culture of methanotrophic bacteria was studied. The substrate factors examined were ammonia, iron, copper, manganese, phosphate, and sulphide. The presence of iron in the growth medium had a strong effect on the yield coefficient. Yield coefficients up to 0.49 mg protein per mg methane were observed when iron was added at concentrations of 0.10–5.0 mg/l. Iron addition also increased the maximum methane utilization rate. The same effect was observed after addition of ammonium to a medium where nitrate was the only nitrogen source. The observed Monod constant for methane utilization increased with increasing concentration of ammonia. This shows that ammonia is a weak competitive inhibitor as observed by other researchers. Relatively high levels of both ammonia (70 mg/l) and copper (300 µg/l) inhibited the methane degradation, probably due to the toxic effect of copper-amine complexes.
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  • 77
    ISSN: 1573-0417
    Keywords: geochemistry ; Guatemala ; Holocene ; lakesediment ; Maya ; magnetic susceptibility ; paleolimnology ; pollen ; stable isotopes
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract We used multiple variables in a sediment core from Lake Peten-Itza, Peten, Guatemala, to infer Holocene climate change and human influence on the regional environment. Multiple proxies including pollen, stable isotope geochemistry, elemental composition, and magnetic susceptibility in samples from the same core allow differentiation of natural versus anthropogenic environmental changes. Core chronology is based on AMS 14C measurement of terrestrial wood and charcoal and thus avoids the vagaries of hard-water-lake error. During the earliest Holocene, prior to ∼9000 14C yr BP, the coring site was not covered by water and all proxies suggest that climatic conditions were relatively dry. Water covered the coring site by ∼9000 14C yr BP, coinciding with filling of other lakes in Peten and farther north on the Yucatan Peninsula. During the early Holocene (∼9000 to ∼6800 14C yr BP), pollen data suggest moist conditions, but high δ 18O values are indicative of relatively high E/P. This apparent discrepancy may be due to a greater fractional loss of the lake's water budget to evaporation during the early stages of lake filling. Nonetheless, conditions were moist enough to support semi-deciduous lowland forest. Decrease in δ 18O values and associated change in ostracod species at ∼6800 14C yr BP suggest a transition to even moister conditions. Decline in lowland forest taxa beginning ∼5780 14C yr BP may indicate early human disturbance. By ∼2800 14C yr BP, Maya impact on the environment is documented by accelerated forest clearance and associated soil erosion. Multiple proxies indicate forest recovery and soil stabilization beginning ∼1100 to 1000 14C yr BP, following the collapse of Classic Maya civilization.
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  • 78
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    Journal of paleolimnology 19 (1998), S. 265-284 
    ISSN: 1573-0417
    Keywords: Holocene ; lacustrine ; sedimentation ; Lake Winnipeg ; sediment cores ; geochemistry ; mineralogy ; texture
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Two seismic facies were recognized in the sedimentary sequence overlying acoustic basement in Lake Winnipeg. The upper facies, which overlies a regional unconformity, is termed the Lake Winnipeg Sequence. Based on the seismostratigraphy, lithostratigraphy, and radiocarbon dates of approximately 4000 and 7000 yr BP from material collected directly over the unconformity in the southern and northern parts of the lake, respectively, this facies has been interpreted as representing Holocene sedimentation. Results of compositional and textural analyses of the Holocene sediment (Winnipeg sediment) from thirteen long (〉2 m) cores indicate a transgressional sequence throughout the basin. In the South Basin, the generally fining upward sequence is characterized at the base by silt-sized detrital carbonate minerals, quartz and feldspar which decrease in concentration upward. In this basin, the high carbonate content and V/Al and Zn/Al ratios are indicative of a Paleozoic and Cretaceous provenance for sediment derived from glacial deposits through shoreline erosion and fluvial transport, via the Red River. Sedimentation in the central part of the lake and the North Basin is attributed to shoreline erosion of sand and gravel beaches. Consequently, the texture of these sediments is generally coarser than in the South Basin, and the composition primarily reflects a Paleozoic and Precambrian provenance. The basin-wide decrease in Ca, total carbonate minerals, dolomite and calcite concentrations upward in the cores is reflected by a decrease in the detrital carbonate component in all but the most northern cores. Other basin-wide trends show an upward increase in organic content in all cores. An increase in grain size near the top of most cores suggests a major, basin-wide change in sedimentation within the last, approximately 900 years in the South Basin.
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  • 79
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    Journal of paleolimnology 20 (1998), S. 135-150 
    ISSN: 1573-0417
    Keywords: geochemistry ; heavy metals ; lake sediments ; palaeolimnology ; Lake Baikal ; Russia
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Geochemical analysis of six radiometrically dated short cores of recent sediment from Lake Baikal shows clear evidence of enhanced Pb supply. However, the sediment concentration increases are very small; the average Pb concentration rises from a baseline value of 10.9 μg g-1 to a peak value of only 14.8 μg g-1. In contrast to the more polluted lakes commonly studied in Europe and North America, variation in Pb concentration is far more strongly influenced by natural variation than by pollution. In sediment deposited over the last 150–200 years 73% of the variance in the sediment Pb concentration can be accounted for by variation in bulk composition of the sediment, and by atmospheric pollution. Factors influencing Pb concentrations over this time period are, in order of decreasing average importance (fraction of total variance explained), catchment supply (indicated by 226Ra activity variation) (43%), anthropogenic Pb emissions (24%), and dilution by ferromanganese hydroxides (6%). On longer (1000s of years) time scales dilution by biogenic silica is probably more important. The recent enhanced supply of catchment Pb correlates with accelerating accumulation rates, indicating a link with enhanced erosion. Anthropogenic sources dominate only in the southern basin, where local fossil-fuel burning industry is situated. The evidence for a local industrial source for the Pb pollution is strengthened by the high correlation between the inventories for Pb and for spheroidal carbonaceous particles. The absence of detectable anthropogenic Pb enrichment in the northern part of the lake suggests that long-distance Pb pollution is small compared with the local natural supply.
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  • 80
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    Journal of paleolimnology 7 (1992), S. 191-214 
    ISSN: 1573-0417
    Keywords: geochemistry ; metals ; lake sediments ; paleolimnology ; United States
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Sediment cores from 30 low-alkalinity lakes in northern New England (NE), New York (NY), the northern Great Lakes States (NGLS) of Minnesota, Michigan, and Wisconsin, and Florida (FL) have been dated by 210Pb and analyzed for water and organic content, eight major elements (Al, Ti, Fe, Mn, Ca, Mg, Na, K) plus four trace metals (Pb, Zn, Cu, and V). Variations in the percentages of major elements through time are dominated by long-term independent variations in the abundance of SiO2, FeO, and to a lesser extent Ca and Al. Additional variations are caused by varying proportions of inorganic matter. Major variations in chemistry are generally unrelated to documented distrubances in the watersheds; most disturbances are minor fires or selective logging. Accelerated accumulation of Pb from atmospheric sources into sediment first occurs in sediment dated between 1800 and 1850 in NY and NE, slightly later in the NGLS region, and about 1900 in FL. Modern accumulation rates in all areas are comparable (ca. 1 to 4 μg cm−2 yr−1). Accumulation rates of Pb in some lakes have declined significantly from 1975 to 1985. Atmospheric deposition of anthropogenic Zn and Cu is also indicated by generally increasing accumulation rates in sediment cores, but the record is not as clear nor are chemical profiles in all lakes parallel to the trends in atmospheric emissions inferred on the basis of fossil fuel consumption, smelting, and other industrial activities. Inter-lake variations in profiles of Cu and Zn are large. Vanadium accumulation rates increase by the 1940s in NY and NE, but not until the 1950s in the NGLS region. This timing correlates with regional trends in the combustion of fuel oil, a major source of atmospheric V. Acidification of some of the lakes is suggested by decreases in the concentration and accumulation rates of Mn, Ca, and Zn in recent sediment, relative to other elements of catchment origin. The decreases generally occur slightly before the onset of acidification as indicated by diatoms. Increased sediment accumulation rates for Fe may indicate the acidification of watershed soils. The use of the accumulation rate of TiO2 as an indicator of rates of erosion and for normalization of trace metal accumulation rates is in question for lakes where the flux of TiO2 from the atmosphere varies and is a significant fraction of the total flux of TiO2 to the sediment.
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  • 81
    ISSN: 1573-0417
    Keywords: lake acidification ; mid-western U.S.A. ; diatoms ; geochemistry ; pollen ; land use
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Paleoecological analyses of sediments from nine northern Great Lakes states (NGLS) lakes reveal small pH changes in seven of these lakes since 1860, four of these being declines. The largest diatom-inferred (DI) pH declines of 0.5 pH units were found in Brown L. and Denton L., Wisconsin. Two other lakes with suspected total alkalinity declines (based on an acidification model and on historical water chemistry, respectively), McNearney L., Michigan, and Camp 12 L., Wisconsin, have not acidified recently according to diatom-inference techniques. Many of the observed trends of increasing pH are coincident with logging; floristic composition of diatom assemblages also changed coincident with fisheries manipulations in some lakes, but these floristic trends did not affect DI pH. Sediment core profiles of Pb, S, and polycyclic aromatic hydrocarbons provide a record of atmospheric deposition of fossil fuel combustion products beginning around the turn of the century; onset is later and accumulation rates are smaller than for other northeastern study regions of the Paleoecological Investigation of Recent Lake Acidification (PIRLA) Project. The response of diatom species to lakewater pH in the NGLS region is very strong and similar to response in other regions. Overall, there is little paleoecological evidence that acidic deposition has caused significant acidification of lakes in the NGLS region.
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  • 82
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    Journal of paleolimnology 4 (1990), S. 219-238 
    ISSN: 1573-0417
    Keywords: saline lakes ; geochemistry ; paleohydrology ; paleoclimate ; Saskatchewan
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract In the western part of the Canadian Prairies, there are thousands of small, closed-basin saline lakes. Most of these lakes are ephemeral, filling with water during the spring and drying completely by late summer. Ceylon Lake, located in southern Saskatchewan, is typical of many of these shallow ephemeral lacustrine basins. The stratigraphic sequence recovered from this salt playa can be subdivided into six distinct facies types: (a) icelaid gravelly clay loam diamicton; (b) fluvial massive bedded to laminated sand; (c) lacustrine laminated calcareous clay and silt; (d) lacustrine laminated gypsiferous clay and silt; (e) lacustrine black, anoxic, nonlaminated, organic-rich mud; and (f) lacustrine salt. The crystalline salt facies, which can be up to 9 meters thick, is comprised mainly of sodium and sodium + magnesium sulfates, with smaller and more variable proportions of other sulfates, halides, carbonates, and insoluble clastic detritus. Although a variety of postdepositional processes have significantly altered the nature and stratigraphic relationships in the basin, the sediment fill does record, in a general way, the fluctuating depositional, hydrological, and geochemical conditions that existed in the basin since deglaciation. The Ceylon Lake basin originated about 15 000 years ago as meltwater from the retreating glacial ice cut a major spillway system in the drift and bedrock. The initial (early Holocene) phases of lacustrine sedimentation in Ceylon Lake occurred in a relatively deep freshwater lake. By about 6000 years B.P., the lake had become much shallower with numerous episodes of complete drying and subaerial exposure. The most recent 5000 years of deposition in the basin have been dominated by evaporite sedimentation. The composition of the soluble salts deposited during this time indicates some degree of cyclic sedimentation superimposed on an overall gradual shift from a sodium dominated brine to one of mixed sodium and magnesium.
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  • 83
    ISSN: 1573-0417
    Keywords: catchment disturbance ; sediment cores ; magnetic minerals ; geochemistry ; pollen ; diatoms ; Morocco
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Paleolimnological techniques for assessing recent drainage basin disturbance are evaluated in three Moroccan lakes with catchments contrasted in terms of land-use and vegetation. Rates of sediment accumulation in the two lakes with agricultural catchments were relatively high (〉1.6 cm yr-1) in the most recent past. Dilution effects prevented core dating by the 210Pb method alone and post-1953 chronologies were constructed by combining 210Pb and 137Cs data. The recent sediment accumulation rate at the currently least disturbed site, where natural Cedrus forest is still abundant, was relatively low (〈0.4 cm yr-1) but has increased since the mid-19th century. Magnetic, geochemical, pollen, and diatom studies of all three lake sediment cores linked with modern field survey data show that soil erosion in the most vegetationally disturbed catchment (Dayat-er-Roumi) has been high throughout the recent past and that intensity peaks are probably associated with wetland drainage operations beginning in the 1940's. At the partially forested site (Dayat Affougah), pre-1950's woodland clearance and other land-use changes are the likely cause of past major soil erosion episodes. The site currently dominated by natural Cedrus forest (Lac Azigza) shows only minor disturbance during the past c. 150 years although a major soil erosion episode occrred in the 17th century. Paleolimnological analysis has clearly demonstrated that major landscape change has occurred at all three sites. However, only at the two sites with catchment cultivation do previously accelerated soil erosion and lake sediment accumulation rates persist to the present. Information essential for formulation of appropriate management plans is presented and the importance of paleolimnology in assessing man-induced lake-catchment disturbance is stressed.
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  • 84
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    Journal of paleolimnology 10 (1994), S. 69-84 
    ISSN: 1573-0417
    Keywords: geochemistry ; salinity ; paleoclimate ; meromixis ; South Dakota
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Medicine Lake is a highly saline, meromictic, magnesium sulfate, closed-basin lake in northeastern South Dakota. The geochemical, mineralogical, and magnetic stratigraphies of sediments deposited from about 10.8 to 4.5 ka B.P. document the evolution of the saline brine in response to climatic change in the early to mid-Holocene. During the spruce occupation of the Medicine Lake catchment (10.8–10.0 ka B.P.), dark-grey massive basal sediments with low total-sulfur and carbonate content, upwardly increasing organic-carbon content, and high magnetic susceptibility were deposited in a deep freshwater lake. As the vegetation in the area changed from spruce to birch to oak and elm and finally to prairie between 10.0 and 9.2 ka B.P., and as the lake became shallow and salinity increased from 〈2 to 〉10%, light-and dark-grey calcareous and organic-carbon-rich banded sediments with low total-sulfur content and low magnetic susceptibility were deposited. Previous studies have shown that during the forest/prairie transition the lake then changed abruptly from fresh to saline as it lost a substantial portion of its volume. During the early prairie period (9.2–5.5 ka B.P.), alternating sections of aragonite-rich laminae and grey massive sediments with high total-sulfur content and multiple gypsum layers were deposited in a meromictic environment under conditions of fluctuating lake levels and salinity. Continued aridity during the mid-Holocene (5.5–4.5 ka B.P.) probably maintained the lake at relatively low levels and high salinity as dark-grey generally massive sediments with moderate total-sulfur, carbonate, and organic-carbon content and no measurable magnetic susceptibility were deposited.
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  • 85
    ISSN: 1573-0417
    Keywords: Florida ; geochemistry ; 210Pb dating ; macrophytes ; nutrients ; paleolimnology ; sediments ; shallow lakes
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract We retrieved four sediment cores from shallow, eutrophic, macrophyte-dominated Orange Lake (A = 51.4 km2, zmax 〈5 m, zmean 〈 2 m), north-central Florida, USA. The 210Pb-dated profiles were used to evaluate spatial and temporal patterns of bulk sediment and nutrient accumulation in the limnetic zone and to infer historical changes in lake trophic state. Bulk density, organic matter, total carbon, total nitrogen, total phosphorus and non-apatite inorganic phosphorus (NAIP) concentrations displayed stratigraphic similarities among three of four cores, as did accumulation rates of bulk sediment, organic matter and nutrients. Accumulation rates were slower at the fourth site. Nutrients showed generally increasing rates of accumulation since the turn of the century. Percentages of periphytic diatom taxa increased progressively in the cores after ~ 1930. Diatom-inferred limnetic total P trends were similar among profiles. Eutrophic conditions were inferred for the period prior to the turn of the century. The lake was hypereutrophic in the early decades of the 1900s, but inferred limnetic total P values declined after ~ 1930. Declining inferred limnetic total P trends for the last 60--70 years were accompanied by concomitant increases in accumulation rates of total P and NAIP on the lake bottom. Several lines of evidence suggest that after ~ 1930, phosphorus entering Orange Lake was increasingly utilized by submersed macrophytes. Paleolimnological records from Orange Lake highlight the importance of using multiple sediment variables to infer past trophic state and suggest that aquatic macrophytes can play a role in regulating water-column nutrient concentrations in shallow, warm-temperate lakes.
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  • 86
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    Keywords: paleolimnology ; geochemistry ; chironomids ; Late glacial - Holocene transition ; Argentina
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Stratigraphy of Lake El Trébol (41°S 71°W, 758 m a.s.l.) described from an 11 m long sediment core provided a continuous record of patecenvironmental changes occurred during the last 14,000 years in southern South America east of the Andes. Located in an ecotonal area within a strong humidity gradient, this lake offers a unique opportunity to develop paleolimnological studies. Using a geochemical approach that includes elemental analysis, bulk organic matter, major nutrients and pigments combined with chironomids and pollen analysis, three zones were identified in the sedimentary record of this take. The oldest one (between 680 and 1,100 cm) corresponds to the late Glacial period. During that time, clayish laminated sediments were formed in a proglacial environment. Low organic matter, biogenic silica and nitrogen contents and the absence of pigments, pollen and chironomids characterise this period. At the end of this period, ca. 14,000 yr BP, a sharp increase in phosphorus concentrations predates major changes in limnological parameters. The transition zone (between 560 and 680 cm) is related to major changes in the drainage system that started soon after ca. 14,000 yr BP and continued to ca. 10,500 yr BP. The chemical composition of the sediments was affected by an increase in physical weathering mechanisms almost coincident with the increase in the regional volcanic activity that produced suspended volcanic detritus. The increase of mainly coarser detritical components may indicate a reorganisation of the fluvial system by that time. Simultaneously, an increase in the productivity of the lake accompanied by a gradual replacement of open vegetation with Nothofagus, Poaceae and Ericaceae, by Nothofagusforest, was observed. In the last zone (between 0 and 560 cm) the productivity of Lake El Trébol achieves maximum values. The trends in geochemical and biological indicators observed at Lake El Trébol can be up to some extent, correlated to those registered in Lake Mascardi. The results support earlier paleoctimatic scenarios from southern South America.
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    Journal of paleolimnology 23 (2000), S. 213-221 
    ISSN: 1573-0417
    Keywords: geochemistry ; heavy metals ; palaeolimnology ; sediment ; soil ; X-ray fluorescence
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Energy dispersive isotope-source X-ray fluorescence (XRF) analysers are little used in academic environmental research, in spite of being ideally suited to a number of tasks. In this paper an XRF method is tested by measuring a wide range of environmental materials of known elemental composition. Precision, accuracy and detection limits are presented. Using isotope-source X-ray fluorescence analysis, the total concentrations of Si, Ti, Ca, K, Fe, Mn, Cl, S, Nb, Ni, Pb, Rb, Sr, Zn and Zr can be determined in soils and sediments at a rate of 〉70 samples per day. The combination of speed and accuracy makes the technique ideal for three classes of application within environmental research. First, in sediments and soils that are highly heterogeneous, reliable characterisation is more dependent upon the number of samples measured than on measurement precision or accuracy. Under these circumstances the method is sufficiently accurate to be used alone. This is also the case where there is high and wide ranging contamination of sediment or soil by Pb and Zn. Second, major elements (Si, Ti, Fe, Ca, K and S) can be measured with sufficient accuracy in sediments and soils to aid the interpretation of other sediment chemical analyses. Third, the technique is ideal for the rapid screening of sediment or soil, allowing effective targeting of samples for more time consuming or expensive analyses. The XRF method presented here offers rapid, non-destructive total elemental analysis of sediments and soils that is sufficiently accurate to be useful in environmental research.
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  • 88
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    Journal of paleolimnology 24 (2000), S. 369-393 
    ISSN: 1573-0417
    Keywords: paleolimnology ; shoreland development ; geochemistry ; diatoms ; eutrophication ; Wisconsin
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Four Wisconsin, USA lakes were examined with paleolimnological techniques to determine the effects of shoreland development on water quality. Geochemical parameters such as aluminum, iron, manganese, phosphorus, nitrogen, and carbon were used to document watershed inputs while redox sensitive elements provided information on changes in hypolimnetic oxygen levels. Changes in the diatom community were used to assess the impacts of development upon the lakes' trophic status as well as changes in the littoral community. We assessed the relative sensitivity of high vs. low ANC lakes. The initial shoreland development, late in the 19th or early in the 20th century, involved seasonal cabins and minimal disturbance of the shoreland. This development phase had minimal impact upon the lakes compared to that during the mid- and late-twentieth century. Increased levels of iron and aluminum indicated the highest input of sediment occurred during the construction phase of converting shoreland homes from seasonal to year-round usage. Phosphorus deposition increased moderately in the high alkalinity lakes but more so in the low alkalinity lakes. In the low alkalinity stratified lake, increased levels of iron and manganese in the last decade indicated more anoxia in the hypolimnion. Phosphorus levels have also increased during this time period most likely as a result of elevated phosphorus release from the sediments. In the high alkalinity lakes, as the nutrient levels increased, diatom production initially shifted from benthic taxa of the family Fragilariaceae to metalimnetic taxa and as nutrients increased further, epilimnetic species. In the low alkalinity lakes, prior to settlement the major site of diatom prodution was the open water. Coincidental with the early shoreland development was an increase of macrophyte density as indicated by the epiphytic diatom Achnanthidium minutissimum ((Kützing) Czarnecki (= Achnanthes minutissima Kützing). The water quality in the high alkalinity lakes showed some improvement following completion of the home construction phase, especially in the lake with lower development density. The low alkalinity lakes did not show improved water quality and appear more sensitive to shoreland development.
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    Journal of paleolimnology 10 (1994), S. 199-212 
    ISSN: 1573-0417
    Keywords: saline lake ; geochemistry ; mineralogy ; lithostratigraphy ; paleolimnology ; Great Plains ; evaporites
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Little Manitou Lake is a topographically closed, hypersaline lake that occupies a long, linear glacial meltwater channel in the northern Great Plains of western Canada. Most of the modern and late Holocene sediment in the lake has been generated from within the basin itself, either by endogenic inorganic precipitation or by other authigenic processes. These endogenic and authigenic precipitates, composed of mainly very soluble sulfate salts and sparingly soluble carbonates, provide an explicit record of the past chemical and hydrological fluctuations that have occurred in the lake. Although detailed chronostratigraphy is incomplete, preliminary14C dating indicates an age of about 2000 years for the oldest sediment recovered from the basin. Five subsurface sedimentary facies are identified in offshore cores. From the base these are: (i) structureless, gray clay, (ii) gypsiferous mud, (iii) structureless, organic-rich mud, (iv) finely laminated aragonitic mud, and (v) Na and Mg sulfate salts. The lithostratigraphy and variation in the mineralogical composition of the sediment indicate that Little Manitou Lake experienced significant water level changes and compositional fluctuations during the past several millennia. The basal clays indicate a relatively deep, freshwater lake existed about 2000 years ago, but was soon followed by a period of low water/playa sedimentation and a negative hydrological budget in the basin. Water levels gradually increased after about 1500 years ago in response to a cooler and wetter climate. This resulted in development of a meromictic, saline to hypersaline lake characterized by periodic carbonate (aragonite) whitings. Water levels again decreased about 1000 years ago, resulting in a breakdown of meromixis and initiation of subaqueous evaporitic salt precipitation. Although the brine in Little Manitou Lake has fluctuated between Na-SO4 and Mg-Na-SO4 -Cl types during the past 1000 years, water levels and overall salinities have remained relatively constant.
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  • 90
    ISSN: 1573-0417
    Keywords: acidification ; geochemistry ; atmospheric loading ; diatoms ; in situ alkalinity ; forest fires
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Paleolimnological methods are combined with statistical multivariate analyses (PCA and CCA) to study the effects of local environmental disturbances and changes in loading of atmospheric origin on water acidity and the physiochemical properties of the sediment in a small, naturally acidic rocky lake in southern Finland. The pH of the lake as calculated from the diatom flora increased by 0.9 pH units as a consequence of a forest fire in the catchment area at the turn of the last century, and the changes in the diatom assemblages point to an increase in dys(eu)trophy and turbulence. In terms of element influx (in µg cm-2 yr-1), the effects of the fire are seen in a slight increase in the accumulation of lithophilous elements. Diatom-inferred pH values decline upwards in the sediment, but do not regain the level recorded before the fire. This is attributed to reactions between Fe3+ and S, which has partly accumulated from the air as SO2-, producing internal alkalinity. Accumulation rates of many elements increase markedly after the 1960s, an effect for Al, Mg, Na, P and Zn may be connected mainly with the enhanced accumulation of dry matter, whereas the accumulation of K, Ni, Pb, Ti and V in surface sediment are obviously related to atmospheric loading. Measured accumulation rates of Cd and Cu are lower than the calculated values especially in the surface sediment, possibly because of diagenetic changes. Accumulation of Ca and Mn decreases towards the surface on account of acidification of anthropogenic origin.
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  • 91
    ISSN: 1573-0417
    Keywords: diatoms ; pollen ; geochemistry ; salinity ; paleoclimate ; South Dakota
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Geosciences
    Notes: Abstract Medicine Lake is a highly saline meromictic lake in eastern South Dakota. A lithostratigraphic and biostratigraphic study of the late-glacial and early post-glacial sediments shows that it was a relatively deep dilute freshwater lake during the period of the Picea pollen zone. When spruce forest changed to a Betula and then to a Quercus/Ulmus woodland in the early post-glacial period, the lake water became more concentrated but remained fresh. However, during the subsequent rapid transition to prairie in the early Holocene, when Gramineae, Ambrosia, and Artemisia dominated dry-land vegetation, the freshwater diatom flora was progressively replaced by a saline assemblage characterized by Cyclotella quillensis, Chaetoceros, and eventually Cyclotella caspia. The lake became permanently saline at about 9000 yr BP. A comparison of the fossil diatom assemblages with surface-sediment samples from a range of lakes in the Dakotas indicates that the change involved an increase in conductivity from about 500 μS cm−1 in the late-glacial period to 〉 10 000 μS cm−1 in the early Holocene. This rapid change is also marked by an abrupt increase in sulphate concentration in the sediment, the first appearance of bands of gypsum crystals, and the beginning of a well-laminated core sequence that continues through the remaining sediment record. Conditions of high salinity have prevailed to the present day.
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    Nutrient cycling in agroecosystems 51 (1998), S. 209-215 
    ISSN: 1573-0867
    Keywords: Desorption ; kinetics ; microbial transformation ; phosphate ; soils
    Source: Springer Online Journal Archives 1860-2000
    Topics: Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition
    Notes: Abstract The improvement of P management in agriculture and environment requires a good understanding of residual effect of applied P in soils. The specific adsorption of P on variable charge minerals has been considered as the major mechanism that leads to a very low utilization of P fertilizer by crops within a growing season in Chinese red soils. Soil incubation and isotope tracing analysis were carried out to examine the transformation kinetics and potential availability of added specifically sorbed 32P in two pH contrasting light textured soils. The 32P recovered by 0.5 M NaHCO3 extraction and microbial biomass-P measurement from the added specifically sorbed 32P in the soils was well described by a first-order reaction and a Langmuir-type kinetic model, with correlation coefficients (R) being, on average, 0.938 and 0.959, respectively. The half-life (t1/2, from the first-order model) of the four tested mineral-P complexes ranged from 29 to 47 d in the acid sandy soil and 33 to 105 d in the neutral silty soil. Goethite-P was the most stable among the four tested mineral-P complexes. The potential availability of the mineral complex P (q m , in percent of total 32P added) obtained from the Langmuir equation ranged from 43.7 to 90.9% for the four mineral-P complexes, and decreased in the order: Al oxide-P (90.9%) 〉 montmorillonite-P (86.2%) 〉 kaolinite-P (77.5%) 〉 goethite-P (60.2%) in the acid sandy soil, whereas the order was Al oxide-P (89.3%) 〉 kaolinite-P (86.2%) 〉 montmorillonite-P (82.6%) 〉 goethite-P (43.7%) in the neutral silty soil. Based on the release rate and potential availability, kaolinite-P and Al oxide-P could be important sources for residual effect of applied P in variable-charge soils. The goethite-P has the lowest release rate and potential availability among the mineral-P complexes, implying that iron oxides may be the most important variable-charge mineral responsible for P fixation in the Chinese red soils.
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    Nutrient cycling in agroecosystems 39 (1994), S. 39-42 
    ISSN: 1573-0867
    Keywords: Controlled release fertilizers ; kinetics ; mechanism ; nutrient supply ; rate of release ; slow release fertilizers (SRF)
    Source: Springer Online Journal Archives 1860-2000
    Topics: Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition
    Notes: Abstract Individual granules within a given granule population of a slow-release fertilizer (SRF) have a different release pattern. The populations studied differed both in relation to the time delay before the start of the release process and to the duration of the release. An association between a short delay period and a rapid release was found. The random reease distribution can be approximated using first-order rate equations. In cases, a term describing a “lag” period should be added. The distribution of release timing among the fertilizer granules may allow a long-lasting nutrient supply to the plant, as long as there are enough granules within the root zone to allow a uniform supply pattern.
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  • 94
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    Antonie van Leeuwenhoek 60 (1991), S. 175-191 
    ISSN: 1572-9699
    Keywords: growing systems ; kinetics ; murein wall ; nucleic acid ; protein ; turnover
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology
    Notes: Abstract Living organisms do not just grow by synthesizing cellular components. As part of the necessary steps for existence, some components are degraded after synthesis. Even for bacteria in balanced, exponential growth some substances, under some conditions, are turned over. In other phases of growth turnover can be much more extensive, but it is still selective. This review covers studies with animals as a way to put the studies on microorganisms in perspective. The history, the mathematics, and experimental design of turnover experiments are reviewed. The important conclusion is that most of the proteins during balanced growth are very stable in bacteria, although ribosomal proteins are degraded under starvation conditions. Another generalization is that the process of wall enlargement in general is associated with obligatory turnover of the peptidoglycan.
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  • 95
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    Journal of statistical physics 95 (1999), S. 23-43 
    ISSN: 1572-9613
    Keywords: model alloy ; Monte Carlo ; elastic interactions ; phase separation ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Physics
    Notes: Abstract We study via Monte Carlo simulations the influence of elastic interactions on the ordering and decomposition of a two-dimensional model binary alloy with antiferromagnetic nearest and ferromagnetic next nearest neighbor type interactions following a quench into the coexistence region. The elastic interaction leads to the development of a platelet morphology for the segregated ordered and disordered regions. A length scale characterizing the coarsening process follows a law of the type R=a+bt 1/3 with the growth b decreasing with the amount of ordered phase; this appears to be due to the presence of anti-phase boundaries between neighboring domains ordered on different sublattices which are difficult to eliminate. The application of uniaxial external stress results in “rafting” of the domains. Many of the simulation results are in agreement with experimentally observed effects in nickel-base superalloys.
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  • 96
    ISSN: 1572-9729
    Keywords: bioavailability ; builders ; detergents ; kinetics ; mineralization ; sewage sludge ; soil
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Energy, Environment Protection, Nuclear Power Engineering , Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition
    Notes: Abstract Tetradecenyl succinic acid (TSA) is the major component of a detergent builder (C12-C14 alkenyl succinic acid), which is inherently biodegradable. 14C-TSA was dosed as a component of sewage sludge into a soil with a history of sludge amendment at final added concentrations of 1.5 and 30 mg (kg soil)-1. In addition, it was dosed to the soil in an aqueous solution to a final added concentration of 30 mg (kg soil)-1. Dose and form were found to have a pronouced effect on the mineralization kinetics. When dosed in a realistic form and concentration (i.e. 1.5 mg (kg soil)-1 as a component of sludge), TSA was mineralized at its highest rate and to its greatest extent, and the mineralization half-life was 2.4 days. When dosed at 30 mg (kg soil)-1 as a component of sludge, mineralization began immediately, and the half-life was 23 days. In contrast, when dosed at this concentration in aqueous solution, the onset of mineralization was preceded by a 13 day lag period and the mineralization half-life was 69 days. Primary biodegradation and mineralization rates of TSA were very similar. Approximately, half the radioactivity was evolved as 14CO2, while the remaining radioactivity became non-extractable, having presumably been incorporated into biomass or natural soil organic matter (humics). This study demonstrated that TSA is effectively removed from sludge-amended soils as a result of biodegradation. Furthermore, it showed the effect that dose form and concentration have on the biodegradation kinetics and the importance of dosing a chemical not only at a relevant concentration but also in the environmental form in which it enters the soil environment.
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  • 97
    ISSN: 1572-9729
    Keywords: bacteria ; degradation ; denitrification ; kinetics ; stoichiometry ; toluene
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Energy, Environment Protection, Nuclear Power Engineering , Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition
    Notes: Abstract Batch experiments were carried out to investigate the stoichiometry and kinetics of microbial degradation of toluene under denitrifying conditions. The inoculum originated from a mixture of sludges from sewage treatment plants with alternating nitrification and denitrification. The culture was able to degrade toluene under anaerobic conditions in the presence of nitrate, nitrite, nitric oxide, or nitrous oxide. No degradation occurred in the absence of Noxides. The culture was also able to use oxygen, but ferric iron could not be used as an electron acceptor. In experiments with14C-labeled toluene, 34%±8% of the carbon was incorporated into the biomass, while 53%±10% was recovered as14CO2, and 6%±2% remained in the medium as nonvolatile water soluble products. The average consumption of nitrate in experiments, where all the reduced nitrate was recovered as nitrite, was 1.3±0.2 mg of nitrate-N per mg of toluene. This nitrate reduction accounted for 70% of the electrons donated during the oxidation of toluene. When nitrate was reduced to nitrogen gas, the consumption was 0.7±0.2 mg per mg of toluene, accounting for 97% of the donated electrons. Since the ammonia concentration decreased during degradation, dissimilatory reduction of nitrate to ammonia was not the reductive process. The degradation of toluene was modelled by classical Monod kinetics. The maximum specific rate of degradation, k, was estimated to be 0.71 mg toluene per mg of protein per hour, and the Monod saturation constant, K s , to be 0.2 mg toluene/l. The maximum specific growth rate, μ max , was estimated to be 0.1 per hour, and the yield coefficient, Y, was 0.14 mg protein per mg toluene.
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  • 98
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    Biodegradation 7 (1996), S. 73-81 
    ISSN: 1572-9729
    Keywords: diesel oil ; biodegradation ; CSTR ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Energy, Environment Protection, Nuclear Power Engineering , Agriculture, Forestry, Horticulture, Fishery, Domestic Science, Nutrition
    Notes: Abstract In batch culture diesel oil was degraded rapidly, with a maximum growth rate (for a consortium of microorganisms) of 0.55 h-1. The corresponding yield Y SX was 0.1 Cmol/Cmol. In a continuous stirred tank reactor the maximum dilution rate was about 0.25 h-1, with a yield of 0.3 Cmol/Cmol. With a residence time of 1 day 82% of the influent oil was degraded. In the batch reactor, of the mixture of linear and branched alkanes the linear alkanes were degraded fastest and with the highest yield. Only after most of the linear alkanes had disappeared were the branched alkanes consumed. In a CSTR a large part of the branched alkanes was not degraded.
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  • 99
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    Cellular and molecular life sciences 41 (1985), S. 1563-1564 
    ISSN: 1420-9071
    Keywords: Cytosine deaminase ; kinetics ; pyrophosphate ; orotidine monophosphate
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Medicine
    Notes: Summary The maximal velocity of the reaction (Vmax) and the half-saturation constant (K0.5) values of theS. typhimurium cytosine deaminase were altered in the presence of its effectors, pyrophosphate and orotidine monophosphate. From the kinetics of orotidine monophosphate inhibition of cytosine deaminase, it was characterized as a mixed-type noncompetitive inhibitor.
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  • 100
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    Cellular and molecular life sciences 47 (1991), S. 1104-1118 
    ISSN: 1420-9071
    Keywords: Transaminase ; decarboxylase ; serine hydroxymethyltransferase ; pyridoxal 5′-phosphate ; enzyme mechanism ; stereochemistry ; kinetics
    Source: Springer Online Journal Archives 1860-2000
    Topics: Biology , Medicine
    Notes: Abstract Pyridoxal 5′-phosphate is a coenzyme for a number of enzymes which catalyse reactions at Cα of amino acid substrates including transaminases, decarboxylases and serine hydroxymethyltransferase. Using the X-ray coordinates for a transaminase, aspartate aminotransferase, and the results of stereochemical and mechanistic studies for decarboxylases and serine hydroxymethyltransferase, an active-site structure for the decarboxylase group is constructed. The structure of the active-site is further refined through active-site pyridoxyllysine peptide sequence comparison and a 3-D catalytic mechanism for the L-α-amino acid decarboxylases is proposed. The chemistry of serine hydroxymethyltransferase is re-examined in the light of the proposed decarboxylase mechanism.
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