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  • Weitere Quellen  (16)
  • ACS (American Chemical Society)  (11)
  • American Chemical Society
  • 2020-2024
  • 2015-2019  (16)
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  • 2017  (16)
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  • 2020-2024
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  • 1
    Publikationsdatum: 2017-11-20
    Beschreibung: Marine methane hydrate in sands has huge potential as an unconventional gas resource; however, no field test of their production potential had been conducted. Here, we report the world’s first offshore methane hydrate production test conducted at the eastern Nankai Trough and show key findings toward future commercial production. Geological analysis indicates that hydrate saturation reaches 80% and permeability in the presence of hydrate ranges from 0.01 to 10 mdarcies. Permeable (1–10 mdarcies) highly hydrate-saturated layers enable depressurization-induced gas production of approximately 20,000 Sm3/D with water of 200 m3/D. Numerical analysis reveals that the dissociation zone expands laterally 25 m at the front after 6 days. Gas rate is expected to increase with time, owing to the expansion of the dissociation zone. It is found that permeable highly hydrate-saturated layers increase the gas–water ratio of the production fluid. The identification of such layers is critically important to increase the energy efficiency and the technical feasibility of depressurization-induced gas production from hydrate reservoirs.
    Materialart: Article , PeerReviewed
    Format: text
    Standort Signatur Erwartet Verfügbarkeit
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  • 2
    Publikationsdatum: 2020-07-27
    Beschreibung: In the colloidal synthesis of iron sulfides, a series of dialkyl disulfides, alkyl thiols, and dialkyl disulfides (allyl, benzyl, tert-butyl, and phenyl) were employed as sulfur sources. Their reactivity was found to tune the phase between pyrite (FeS2), greigite (Fe3S4), and pyrrhotite (Fe7S8). DFT was used to show that sulfur-rich phases were favored when the C–S bond strength was low in the organosulfurs, yet temperature dependent studies and other observations indicated the reasons for phase selectivity were more nuanced; the different precursors decomposed through different reaction mechanisms, some involving the oleylamine solvent. The formation of pyrite from diallyl disulfide was carefully studied as it was the only precursor to yield FeS2. Raman spectroscopy indicated that FeS2 forms directly without an FeS intermediate, unlike most synthetic procedures to pyrite. Diallyl disulfide releases persulfide (S–S)2– due to the lower C–S bond strength relative to the S–S bond strength, as well as facile decomposition in the presence of amines through SN2′ mechanisms at elevated temperatures.
    Materialart: Article , PeerReviewed
    Format: text
    Standort Signatur Erwartet Verfügbarkeit
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  • 3
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    ACS (American Chemical Society)
    In:  Environmental Science & Technology, 51 (12). pp. 7036-7046.
    Publikationsdatum: 2020-07-31
    Beschreibung: Microplastic fibers make up a large proportion of microplastics found in the environment, especially in urban areas. There is good reason to consider synthetic textiles a major source of microplastic fibers, and it will not diminish since the use of synthetic fabrics, especially polyester, continues to increase. In this study we provide quantitative data regarding the size and mass of microplastic fibers released from synthetic (polyester) textiles during simulated home washing under controlled laboratory conditions. Consideration of fabric structure and washing conditions (use of detergents, temperature, wash duration, and sequential washings) allowed us to study the propensity of fiber shedding in a mechanistic way. Thousands of individual fibers were measured (number, length) from each wash solution to provide a robust data set on which to draw conclusions. Among all the variables tested, the use of detergent appeared to affect the total mass of fibers released the most, yet the detergent composition (liquid or powder) or overdosing of detergent did not significantly influence microplastic release. Despite different release quantities due to the addition of a surfactant (approximately 0.025 and 0.1 mg fibers/g textile washed, without and with detergent, respectively), the overall microplastic fiber length profile remained similar regardless of wash condition or fabric structure, with the vast majority of fibers ranging between 100 and 800 μm in length irrespective of wash cycle number. This indicates that the fiber staple length and/ or debris encapsulated inside the fabric from the yarn spinning could be directly responsible for releasing stray fibers. This study serves as a first look toward understanding the physical properties of the textile itself to better understand the mechanisms of fiber shedding in the context of microplastic fiber release into laundry wash water.
    Materialart: Article , PeerReviewed
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  • 4
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    ACS (American Chemical Society)
    In:  Environmental Science & Technology, 51 (21). pp. 12246-12253.
    Publikationsdatum: 2020-07-31
    Beschreibung: A substantial fraction of marine plastic debris originates from land-based sources and rivers potentially act as a major transport pathway for all sizes of plastic debris. We analyzed a global compilation of data on plastic debris in the water column across a wide range of river sizes. Plastic debris loads, both microplastic (particles 〈5 mm) and macroplastic (particles 〉5 mm) are positively related to the mismanaged plastic waste (MMPW) generated in the river catchments. This relationship is nonlinear where large rivers with population-rich catchments delivering a disproportionately higher fraction of MMPW into the sea. The 10 top-ranked rivers transport 88-95% of the global load into the sea. Using MMPW as a predictor we calculate the global plastic debris inputs form rivers into the sea to range between 0.41 and 4 X 106 t/y. Due to the limited amount of data high uncertainties were expected and ultimately confirmed. The empirical analysis to quantify plastic loads in rivers can be extended easily by additional potential predictors other than MMPW, for example, hydrological conditions.
    Materialart: Article , PeerReviewed
    Format: text
    Format: archive
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  • 5
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    ACS (American Chemical Society)
    In:  Environmental Science & Technology, 51 (14). pp. 7963-7971.
    Publikationsdatum: 2020-07-31
    Beschreibung: Recent studies suggest size-selective removal of small plastic particles from the ocean surface, an observation that remains unexplained. We studied one of the hypotheses regarding this size-selective removal: the formation of a biofilm on the microplastics (biofouling). We developed the first theoretical model that is capable of simulating the effect of biofouling on the fate of microplastic. The model is based on settling, biofilm growth, and ocean depth profiles for light, water density, temperature, salinity, and viscosity. Using realistic parameters, the model simulates the vertical transport of small microplastic particles over time, and predicts that the particles either float, sink to the ocean floor, or oscillate vertically, depending on the size and density of the particle. The predicted size-dependent vertical movement of microplastic particles results in a maximum concentration at intermediate depths. Consequently, relatively low abundances of small particles are predicted at the ocean surface, while at the same time these small particles may never reach the ocean floor. Our results hint at the fate of “lost” plastic in the ocean, and provide a start for predicting risks of exposure to microplastics for potentially vulnerable species living at these depths.
    Materialart: Article , PeerReviewed
    Format: text
    Standort Signatur Erwartet Verfügbarkeit
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  • 6
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    ACS (American Chemical Society)
    In:  Environmental Science & Technology, 51 (8). pp. 4368-4376.
    Publikationsdatum: 2020-07-31
    Beschreibung: It is important to understand the fragmentation processes and mechanisms of plastic litter to predict microplastic production in the marine environment. In this study, accelerated weathering experiments were performed in the laboratory, with ultraviolet (UV) exposure for up to 12 months followed by mechanical abrasion (MA) with sand for 2 months. Fragmentation of low-density polyethylene (PE), polypropylene (PP), and expanded polystyrene (EPS) was evaluated under conditions that simulated a beach environment. PE and PP were minimally fragmented by MA without photooxidation by UV (8.7 ± 2.5 and 10.7 ± 0.7 particles/pellet, respectively). The rate of fragmentation by UV exposure duration increased more for PP than PE. A 12-month UV exposure and 2-month MA of PP and PE produced 6084 ± 1061 and 20 ± 8.3 particles/pellet, respectively. EPS pellets were susceptible to MA alone (4220 ± 33 particles/pellet), while the combination of 6 months of UV exposure followed by 2 months of MA produced 12,152 ± 3276 particles/pellet. The number of fragmented polymer particles produced by UV exposure and mechanical abrasion increased with decreasing size in all polymer types. The size-normalized abundance of the fragmented PE, PP, and EPS particles according to particle size after UV exposure and MA was predictable. Up to 76.5% of the initial EPS volume was unaccounted for in the final volume of pellet produced particle fragments, indicating that a large proportion of the particles had fragmented into undetectable submicron particles.
    Materialart: Article , PeerReviewed
    Format: text
    Standort Signatur Erwartet Verfügbarkeit
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  • 7
    Publikationsdatum: 2020-02-06
    Beschreibung: Chemical investigation of the marine sponge Ircinia oros yielded four linear furanosesterterpenoids, including the known metabolites ircinin-1 (1) and ircinin-2 (2) and two new compounds, ircinialactam E (3) and ircinialactam F (4). Their chemical structures were elucidated by using a combination of [α]D, NMR, HRMS, and FT-IR spectroscopy. The absolute configuration of C-18 in compounds 1–3 was identified as R by electronic circular dichroism (ECD) spectroscopy coupled with time-dependent density functional theory calculations. Compounds 1–4 showed moderate leishmanicidal, trypanocidal, and antiplasmodial activities (IC50 values 28–130 μM). This is the second report of rare glycinyl lactam derivatives 3 and 4 from the genus Ircinia.
    Materialart: Article , PeerReviewed
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  • 8
    Publikationsdatum: 2020-02-06
    Beschreibung: Shallow gas migration along hydrocarbon wells constitutes a potential methane emission pathway that currently is not recognized in any regulatory framework or greenhouse gas inventory. Recently, the first methane emission measurements at three abandoned offshore wells in the Central North Sea (CNS) were conducted showing that considerable amounts of biogenic methane originating from shallow gas accumulations in the overburden of deep reservoirs were released by the boreholes. Here, we identify numerous wells poking through shallow gas pockets in 3D seismic data of the CNS indicating that about one third of the wells may leak, potentially releasing a total of 3-17 kt of methane per year into the North Sea. This poses a significant contribution to the North Sea methane budget. A large fraction of this gas (~42 %) may reach the atmosphere via direct bubble transport (0-2 kt yr-1) and via diffusive exchange of methane dissolving in the surface mixed layer (1-5 kt yr-1), as indicated by numerical modeling. In the North Sea and in other hydrocarbon-prolific provinces of the world shallow gas pockets are frequently observed in the sedimentary overburden and aggregate leakages along the numerous wells drilled in those areas may be significant.
    Materialart: Article , PeerReviewed , info:eu-repo/semantics/article
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  • 9
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    American Chemical Society
    In:  The Journal of Organic Chemistry, 82 (1). pp. 269-275.
    Publikationsdatum: 2020-01-02
    Beschreibung: A synthesis of the 12,12′-azo-analogue of ritterazine N from hecogenin is reported. Ring contraction of two 6/5 bicyclic ring systems, one trans-fused and another spiro, to 5/5 spiro ring systems is accomplished with excellent stereochemical control. Key transformations include an abnormal Baeyer–Villiger oxidation, a Norrish type I cleavage, an intramolecular dipolar [3 + 2] cycloaddition, and an intramolecular oxymecuration. Failing to uncover the β-OH ketone from the isoxazoline ring, we end up with a synthesis of a cyclic analogue of ritterazine N.
    Materialart: Article , PeerReviewed
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  • 10
    Publikationsdatum: 2020-12-04
    Beschreibung: Nanoscale ternary chalcogenides have attracted intense research interest due to their wealth of tunable properties and diverse applications in energy and environmental and biomedical fields. In this article, ultrasmall magnetic CuFeSe2 ternary nanocrystals (〈5.0 nm) were fabricated in the presence of thiol-functionalized poly(methacrylic acid) by an environmentally friendly aqueous method under ambient conditions. The small band gap and the existence of intermediate bands lead to a broad NIR absorbance in the range of 500-1100 nm and high photothermal conversion efficiency (82%) of CuFeSe2 nanocrystals. The resultant CuFeSe2 nanocrystals show superparamagnetism and effective attenuation for X-rays. In addition, they also exhibit excellent water solubility, colloidal stability, biocompatibility, and multifunctional groups. These properties enable them to be an ideal nanotheranostic agent for multimodal imaging [e.g., photoacoustic imaging (PAI), magnetic resonance imaging (MRI), computed tomography (CT) imaging] guided photothermal therapy of cancer.
    Materialart: Article , PeerReviewed
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