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  • 1
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    Springer
    Publication Date: 2011-06-10
    Description:    We investigate the potential role of dolomite as a long-term buffer on Phanerozoic seawater composition. Using a comprehensive model of Phanerozoic geochemical cycling, we show how variations in the formation rate of sedimentary marine dolomite have buffered seawater saturation state. The total inventory of inorganic carbon reflects the sum of fluxes derived from continental weathering, basalt-seawater exchange, alumino-silicate diagenesis (reverse weathering), and global deposition of calcium carbonate. Although these fluxes are approximately balanced, model results indicate that seawater saturation state is sensitive to the marine dolomite depositional flux. This conclusion is consistent with and constrained by independent proxy data for seawater ion ratios, paleo-atmospheric CO 2 concentrations, and paleo-pH data, and dolomite mass-age distribution through Phanerozoic time. Abundant research indicates that dolomite’s occurrence in marine sediments is sensitive to many factors: temperature, seawater composition, paleogeographic setting, continental organization, etc. Although the complexity of the process of dolomite formation prevents a complete understanding of the relative role of these factors, our model results clearly underscore the importance of this mineral in the chemical history of Phanerozoic seawater. Content Type Journal Article Pages 1-13 DOI 10.1007/s10498-011-9130-7 Authors Rolf S. Arvidson, Department of Earth Science MS-126, Rice University, P.O. Box 1892, Houston, TX 77251-1892, USA Michael W. Guidry, Department of Oceanography, University of Hawaii at Manoa, Honolulu, HI 96822, USA Fred T. Mackenzie, Department of Oceanography, University of Hawaii at Manoa, Honolulu, HI 96822, USA Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 2
    Publication Date: 2011-06-10
    Description:    A new sediment profile imaging (SPI) instrument, CHEM-SPI, was developed for in situ two-dimensional measurements of biogeochemical solutes using fluorosensor foils in sediments and overlying waters. The CHEM-SPI system was used to simultaneously measure vertical sections of pH, O 2 , and p CO 2 distributions in subtidal, surface deposits of Long Island Sound, NY. Images are readily obtained in 5–15 min with inexpensive LED excitation and commercial grade digital cameras having typical pixel resolution of ~50–100 μm over areas 〉150 cm 2 sediment. Seasonal examples of in situ deployments of the instrument revealed extensive horizontal and vertical heterogeneity of pH distributions. pH dynamics were associated with complex biogenic structures in the upper few centimeters of marine sediment and the pulsed input of organic matter during the spring bloom period. The pH beneath the sediment–water interface was dramatically depressed by the bloom input of organic matter but macrofaunal activity otherwise dominated pH variations in the bioturbated zone. The CHEM-SPI system allows direct quantitative confirmation of biogeochemical patterns previously inferred qualitatively from color patterns in visible SPI images. The instrument is sufficiently adaptable in design to accommodate new optical sensor foils for other chemical variables. Content Type Journal Article Pages 1-15 DOI 10.1007/s10498-011-9124-5 Authors Yanzhen Fan, School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000, USA Qingzhi Zhu, School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000, USA Robert C. Aller, School of Marine and Atmospheric Sciences, Stony Brook University, Stony Brook, NY 11794-5000, USA Donald C. Rhoads, 22 Widgeon Road, Falmouth, MA 02540, USA Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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    Topics: Chemistry and Pharmacology , Geosciences
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  • 3
    Publication Date: 2011-06-10
    Description:    The average composition of natural waters such as rivers, lakes, ocean, and hydrothermal vents and corresponding solids in equilibrium (e.g., river-suspended particles or shale; lake sediments; oceanic pelagic clay, organisms, and manganese nodules; and the mid-ocean ridge basalts) do not change randomly. The observed positive correlation between the electron binding energy ( I z [* I z ]) and logarithms of bulk distribution coefficient (log K d ) for cations with charge of 1–4, and the negative correlation between I z [* I z ] and log K d for anions in various aquatic systems are consistent with the prediction from the surface complexation model. In other words, the bond strength between the adsorbed cation and the surface oxygen of hydrated metal oxides, and between the oxygen of adsorbed oxyanion and the surface metal of hydrated metal oxides control the partition of elements between solid and associated liquid in natural aquatic systems. For Mn, Co, Ce, Pb, and Tl, the oxidative uptake at the solid–water interface in the ocean is an additional important process. For alkali and alkaline-earth cations with large ionic radius (such as Cs, Rb, K, and Ba), their relatively small secondary solvation energy further enhances their adsorption onto solid particles. For living and non-living organic matter, the adsorbed B-type cations form extra strong bindings with hydrophilic functional groups such as –SH and –NH 2 on organic matter surface. Content Type Journal Article Pages 1-29 DOI 10.1007/s10498-011-9121-8 Authors Yuan-Hui Li, Department of Oceanography, University of Hawaii at Manoa, Honolulu, HI 96822, USA Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 4
    Publication Date: 2011-06-10
    Description:    Plasmid DNA was incubated at 25°C with aqueous solutions of dissolved Fe(II), S(-II), and nanoparticulate FeS with a mackinawite structure, FeS m . At ≥0.1 mM total dissolved Fe(II) and S(-II), an increase in the proportion of the relaxed plasmid DNA occurs, through scission of the DNA backbone. In solutions where FeS m was precipitated, nanoparticulate FeS m binds to the DNA molecules. In solutions with concentrations below the FeS m solubility product, nicking of supercoiled pDNA occurs. Plasmid DNA appears to be a sensitive proxy for radical reactions. The reactant is proposed to be a sulfur-based radical produced from the iron-catalyzed decomposition of bisulfide, in a manner analogous to the Fenton reaction. This is further supported by experiments that suggest that sulfide free radicals are produced during the photolysis of aqueous solutions of polysulfides. Supercoiling of DNA affects nearly all DNA–protein transactions so the observation of relaxation of supercoiled forms through reaction with FeS solutions has direct implications to biochemistry. The results of this experimentation suggest that genotoxicity in FeS-rich systems is a further contributory factor to the limited survival of organisms in sulfidic environments. Mutations resulting from the interactions of organisms and mobile elements, such as plasmids, in sediments will also be affected in sulfide-rich environments. Content Type Journal Article Pages 1-22 DOI 10.1007/s10498-010-9116-x Authors D. Rickard, School of Earth and Ocean Sciences, Cardiff University, Cardiff, CF103YE UK B. Hatton, School of Earth and Ocean Sciences, Cardiff University, Cardiff, CF103YE UK D. M. Murphy, School of Chemistry, Cardiff University, Cardiff, CF103YE UK I. B. Butler, School of Geosciences, University of Edinburgh, Edinburgh, EH9 3JW UK A. Oldroyd, School of Earth and Ocean Sciences, Cardiff University, Cardiff, CF103YE UK A. Hann, School of Biosciences, Cardiff University, Cardiff, CF103YE UK Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 5
    Publication Date: 2011-06-10
    Description:    At constant temperature, the density of deep waters in the oceans is higher than that of surface waters due to the oxidation of plant material that adds NO 3 , PO 4 , and Si(OH) 4 , and the dissolution of CaCO 3 (s) that adds Ca 2+ and HCO 3 . These increases in the density have been used to estimate the absolute salinity of seawater that is needed to determine its thermodynamic properties. Density (ρ), total alkalinity (TA), and dissolved organic carbon (DOC) measurements were taken on waters collected in the eastern Arctic Ocean. The results were examined relative to the properties of North Atlantic Waters. The excess densities (Δρ = ρ Meas  − ρ Calc ) in the surface Arctic waters were higher than expected (maximum of 0.008 kg m −3 ) when compared to Standard Seawater. This excess is due to the higher values of the normalized total alkalinity (NTA = TA * 35/S) (up to ~2,650 μmol kg −1 ) and DOC (up to ~130 μmol kg −1 ) resulting from river water input. New measurements are needed to determine how the DOC in the river waters contributes to the TA of the surface waters. The values of Δρ in deep waters are slightly lower (−0.004 ± 0.002 kg m −3 ) than that in Standard Seawater. The deep waters in the Arctic Ocean, unlike the Atlantic, Pacific, Indian, and Southern Oceans, do not have significant concentrations of silicate (maximum ~15 μmol kg −1 ) and that can affect the densities. Since the NTA of the deep Arctic waters (2,305 ± 6 μmol kg −1 ) is the same as Standard Seawater (2,306 ± 3 μmol kg −1 ), the decrease in the density may be caused by the lower concentrations of DOC in the deep waters (44–50 μmol kg −1 compared to the Standard Seawater value of 57 ± 2 μmol kg −1 ). The relative deficit of DOC (7–13 μmol kg −1 ) in the deep Arctic waters appears to cause the lower densities (−0.004 kg m −3 ) and Absolute Salinities ( S A , −0.004 g kg −1 ). The effect of increases or decreases in Δρ and δ S A due to DOC in other deep ocean waters may be hidden in the correlations of the changes with silicate. Further work is needed to separate the effects of SiO 2 and DOC on the density of deep waters of the world oceans. Content Type Journal Article Pages 1-16 DOI 10.1007/s10498-010-9111-2 Authors Frank J. Millero, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL 33149, USA Fen Huang, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL 33149, USA Ryan J. Woosley, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL 33149, USA Robert T. Letscher, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL 33149, USA Dennis A. Hansell, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, FL 33149, USA Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 6
    Publication Date: 2011-06-10
    Description:    The paired chemical reactions, Ca 2+  + 2HCO 3 −  ↔ CaCO 3  + CO 2  + H 2 O, overestimate the ratio of CO 2 flux to CaCO 3 flux during the precipitation or dissolution of CaCO 3 in seawater. This ratio, which has been termed ψ, is about 0.6 in surface seawater at 25°C and at equilibrium with contemporary atmospheric CO 2 and increases towards 1.0 as seawater cools and pCO 2 increases. These conclusions are based on field observations, laboratory experiments, and equilibrium calculations for the seawater carbonate system. Yet global geochemical modeling indicates that small departures of Ψ from 1.0 would cause dramatic, rapid, and unrealistic change in atmospheric CO 2 . Ψ can be meaningfully calculated for a water sample whether or not it is in equilibrium with the atmosphere. The analysis presented here demonstrates that the atmospheric CO 2 balance can be maintained constant with respect to seawater CaCO 3 reactions if one considers the difference between CaCO 3 precipitation and burial and differing values for ψ (both 〈1.0) in regions of precipitation and dissolution within the ocean. Content Type Journal Article Pages 1-11 DOI 10.1007/s10498-010-9109-9 Authors Stephen V. Smith, Centro de Investigación Científica y de Educación Superior de Ensenada (CICESE), Ensenada, Baja California México Jean-Pierre Gattuso, INSU-CNRS, Laboratoire d’Océanographie de Villefranche, B.P. 28, 06234 Villefranche-sur-mer, Cedex France Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 7
    Publication Date: 2011-06-10
    Description:    Total trace metals (Cd, Co, Cu, Fe, Mn, Ni, Pb, Zn), Al, and pyrite- and reactive-associated metals were measured for the first time in a microbial mat and its underlying anoxic-sulfidic sediment collected in the saltern of Guerrero Negro (GN), Baja California Sur, Mexico. It is postulated that the formation of acid volatile sulfide (AVS) and pyrite in the area of GN could be limited by the availability of reactive Fe, as suggested by its limited abundance (mat and sediment combined average value of only 19 ± 10 μmol g −1 ; n  = 22) as well as the low pyrite (0.89–7.9 μmol g −1 ) and AVS (0.19–21 μmol g −1 ) concentrations (for anoxic-sulfidic sediments), intermediate degrees of pyritization (12–50%), high degrees of sulfidization (14–100%), generally low degrees of trace metal pyritization, and slight impoverishment in total Fe. This is a surprising result considering the large potential reservoir of available Fe in the surrounding desert. Our findings suggest that pyrite formation in the cycling of trace metals in the saltern of GN is not very important and that other sedimentary phases (e.g., organic matter, carbonates) may be more important reservoirs of trace elements. Enrichment factors [EF Me  = (Me/Al) sample /(Me/Al) background ] of Co, Pb, and Cd were high in the mat (EF Me  = 2.2 ± 0.4, 2.8 ± 1.6 and 34.5 ± 9.8, respectively) and even higher in the underlying sediment (EF Me  = 4.7 ± 1.5, 14.5 ± 6.2 and 89 ± 27, respectively), but Fe was slightly impoverished (average EF Fe of 0.49 ± 0.13 and 0.50 ± 0.27 in both mat and sediment). Organic carbon to pyrite-sulfur (C/S) molar ratios measured in the mat (2.9 × 10 2 –27 × 10 2 ) and sediment (0.81 × 10 2 –6.6 × 10 2 ) were, on average, approximately 77 times higher than those typically found in marine sediments (7.5 ± 2.1). These results may indicate that ancient evaporation basins or hypersaline sedimentary environments could be identified on the basis of extremely high C/S ratios (e.g., 〉100) and low reactive Fe. Content Type Journal Article Pages 1-26 DOI 10.1007/s10498-011-9126-3 Authors Miguel Angel Huerta-Diaz, Instituto de Investigaciones Oceanológicas, Universidad Autónoma de Baja California, Campus Ensenada, Km. 103, Carr. Tijuana-Ensenada, Ensenada, Baja California, Mexico Francisco Delgadillo-Hinojosa, Instituto de Investigaciones Oceanológicas, Universidad Autónoma de Baja California, Campus Ensenada, Km. 103, Carr. Tijuana-Ensenada, Ensenada, Baja California, Mexico X. L. Otero, Departamento de Edafoloxía e Química Agrícola, Facultade de Bioloxía Universidade de Santiago de Compostela, 15782 Santiago de Compostela, Spain José Antonio Segovia-Zavala, Instituto de Investigaciones Oceanológicas, Universidad Autónoma de Baja California, Campus Ensenada, Km. 103, Carr. Tijuana-Ensenada, Ensenada, Baja California, Mexico J. Martin Hernandez-Ayon, Instituto de Investigaciones Oceanológicas, Universidad Autónoma de Baja California, Campus Ensenada, Km. 103, Carr. Tijuana-Ensenada, Ensenada, Baja California, Mexico Manuel Salvador Galindo-Bect, Instituto de Investigaciones Oceanológicas, Universidad Autónoma de Baja California, Campus Ensenada, Km. 103, Carr. Tijuana-Ensenada, Ensenada, Baja California, Mexico Enrique Amaro-Franco, Posgrado en Oceanografía Costera, Facultad de Ciencias Marinas/Instituto de Investigaciones Oceanológicas, Universidad Autónoma de Baja California, Campus Ensenada, Km. 103, Carr. Tijuana-Ensenada, Ensenada, Baja California, Mexico Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 8
    Publication Date: 2011-06-10
    Description:    A field and laboratory study of the accuracy of a method commonly used to determine free sulphide concentrations in the porewater of marine sediments is presented. The method uses an ion-selective electrode (ISE), sensitive to the sulphide ion (S 2− ), in sediments buffered to high pH (〉12) and is commonly used in regulatory monitoring programs to assess the impacts of open net-pen finfish aquaculture on local marine habitats. Here we report that on the timescale of field measurements, the accepted protocol can lead to significant bias of free sulphide measurements, with orders of magnitude higher concentration detected in the buffered sediment–porewater slurry than in porewater samples isolated and analysed separately. Laboratory experiments with model marine sediments and analysis of sediment composition indicate that this bias is likely introduced by the dissolution of particulate sulphides and/or sulphur present in the sediments under the intense alkaline conditions of the protocol. Recommendations for the modification and continued use of this commonly applied field methodology are discussed. Content Type Journal Article Pages 1-19 DOI 10.1007/s10498-011-9137-0 Authors Kristina A. Brown, University of Victoria, School of Earth and Ocean Sciences, Bob Wright Centre, Victoria, BC, Canada Eric R. McGreer, Environmental Protection Division, British Columbia Ministry of Environment, Nanaimo, BC V9T 6J9, Canada Bernie Taekema, Environmental Protection Division, British Columbia Ministry of Environment, Nanaimo, BC V9T 6J9, Canada Jay T. Cullen, University of Victoria, School of Earth and Ocean Sciences, Bob Wright Centre, Victoria, BC, Canada Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 9
    Publication Date: 2011-06-10
    Description:    Hypoxia has been observed in Hood Canal, Puget Sound, WA, USA since the 1970s. Four long sediment cores were collected in 2005 and age-dated to resolve natural and post-urbanization signatures of hypoxia and organic matter (OM) sources in two contrasting basins of Puget Sound: Main Basin and Hood Canal. Paleoecological indicators used for sediment reconstructions included pollen, stable carbon and nitrogen isotopes (δ 13 C and δ 15 N), biomarkers of terrestrial OM (TOM), biogenic silica (BSi), and redox-sensitive metals (RSM). The sedimentary reconstructions illustrated a gradient in RSM enrichment factors as Hood Canal 〉 Main Basin, southern 〉 northern cores, and pre-1900s 〉 1900–2005. The urbanization of Puget Sound watersheds during the 1900s was reflected as shifts in all the paleoecological signatures. Pollen distributions shifted from predominantly old growth conifer to successional alder, dominant OM signatures recorded a decrease in the proportion of marine OM (MOM) concomitant with an increase in the proportion of TOM, and the weight % of BSi decreased. However, these shifts were not coincidental with an overall increase in the enrichment of RSM or δ 15 N signatures indicative of cultural eutrophication. The increased percentage of TOM was independently verified by both the elemental ratios and lignin yields. In addition, isotopic signatures, BSi, and RSMs all suggest that OM shifts may be due to a reduction in primary productivity rather than an increase in OM regeneration in the water column or at the sediment/water interface. Therefore, the reconstructions suggested the Hood Canal has been under a more oxygenated “stance” during the twentieth century compared to prior periods. However, these 2005 cores and their resolutions do not encompass the period of high resolution water column measurements that showed short-lived hypoxia events and fish kills in Hood Canal during the early twenty-first century. The decoupling between the increased watershed-scale anthropogenic alterations recorded in the OM signatures and the relatively depleted RSM during the twentieth century suggests that physical processes, such as deep-water ventilation, may be responsible for the historical variation in oxygen levels. Specifically, climate oscillations may influence the ventilation and/or productivity of deep water in Puget Sound and particularly their least mixed regions. Content Type Journal Article Pages 1-26 DOI 10.1007/s10498-011-9129-0 Authors Jill M. Brandenberger, Pacific Northwest National Laboratory, Battelle Marine Science Laboratory, 1529 West Sequim Bay Road, Sequim, WA 98382, USA Patrick Louchouarn, Departments of Oceanography and Marine Sciences, Texas A&M University, College Station, TX, USA Eric A. Crecelius, Pacific Northwest National Laboratory, Battelle Marine Science Laboratory, 1529 West Sequim Bay Road, Sequim, WA 98382, USA Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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  • 10
    Publication Date: 2011-06-10
    Description:    The sulfide (H 2 S/HS − ) that is emitted from hydrothermal vents begins to oxidize abiotically with oxygen upon contact with ambient bottom water, but the reaction kinetics are slow. Here, using in situ voltammetry, we report detection of the intermediate sulfur oxidation products polysulfides [ \text S \text x 2 - ] and thiosulfate [ \text S 2 \text O 3 2 - ], along with contextual data on sulfide, oxygen, and temperature. At Lau Basin in 2006, thiosulfate was identified in less than one percent of approximately 10,500 scans and no polysulfides were detected. Only five percent of 11,000 voltammetric scans taken at four vent sites at Lau Basin in May 2009 show either thiosulfate or polysulfides. These in situ data indicate that abiotic sulfide oxidation does not readily occur as H 2 S contacts oxic bottom waters. Calculated abiotic potential sulfide oxidation rates are 〈10 −3  μM/min and are consistent with slow oxidation and the observed lack of sulfur oxidation intermediates. It is known that the thermodynamics for the first electron transfer step for sulfide and oxygen during sulfide oxidation in these systems are unfavorable, and that the kinetics for two electron transfers are not rapid. Here, we suggest that different metal catalyzed and/or biotic reaction pathways can readily produce sulfur oxidation intermediates. Via shipboard high-pressure incubation experiments, we show that snails with chemosynthetic endosymbionts do release polysulfides and may be responsible for our field observations of polysulfides. Content Type Journal Article Pages 1-19 DOI 10.1007/s10498-011-9136-1 Authors Amy Gartman, School of Marine Science and Policy, College of Earth, Ocean and Environment, University of Delaware, Lewes, DE 19958, USA Mustafa Yücel, School of Marine Science and Policy, College of Earth, Ocean and Environment, University of Delaware, Lewes, DE 19958, USA Andrew S. Madison, School of Marine Science and Policy, College of Earth, Ocean and Environment, University of Delaware, Lewes, DE 19958, USA David W. Chu, Department of Chemistry and Biochemistry, School of Marine Science and Policy, College of Earth, Ocean and Environment, University of Delaware, Lewes, DE 19958, USA Shufen Ma, School of Marine Science and Policy, College of Earth, Ocean and Environment, University of Delaware, Lewes, DE 19958, USA Christopher P. Janzen, Department of Chemistry, Susquehanna University, Selinsgrove, PA 17870, USA Erin L. Becker, Biology Department, Penn State University, University Park, PA 16801, USA Roxanne A. Beinart, Department of Organismic & Evolutionary Biology, Harvard University, Cambridge, MA 02138, USA Peter R. Girguis, Department of Organismic & Evolutionary Biology, Harvard University, Cambridge, MA 02138, USA George W. Luther, School of Marine Science and Policy, College of Earth, Ocean and Environment, University of Delaware, Lewes, DE 19958, USA Journal Aquatic Geochemistry Online ISSN 1573-1421 Print ISSN 1380-6165
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