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1.
Seven sediment cores were taken in the Sea of Okhotsk in a south-north transect along the slope of Sakhalin Island. The retrieved anoxic sediments and pore fluids were analyzed for particulate organic carbon (POC), total nitrogen, total sulfur, dissolved sulfate, sulfide, methane, ammonium, iodide, bromide, calcium, and total alkalinity. A novel method was developed to derive sedimentation rates from a steady-state nitrogen mass balance. Rates of organic matter degradation, sulfate reduction, methane turnover, and carbonate precipitation were derived from the data applying a steady-state transport-reaction model. A good fit to the data set was obtained using the following new rate law for organic matter degradation in anoxic sediments:
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2.
Complex investigations of recent and Drevnechernomorian (ancient Black Sea) sediments from the outer shelf, continental slope, and deep-water basin of the Russian Black Sea sector have been carried out using samples collected during cruise of the R/V Professor Shtokman organized by the Institute of Oceanology of the Russian Academy of Sciences (March 2009) and expedition of “YUZHMORGEO” (summer 2006). Rates of the main anaerobic processes during diagenesis (sulfate reduction, dark CO2 fixation, methanogenesis, and methane oxidation) were studied for the first time in sediment cores of the studied area. Two peaks in the rate of microbial processes and two sources of these processes were identified: the upper peak near the water-sediment contact is related to the solar energy (OM substrate of the water column) and the lower peak at the base of the Drevnechernomorian sediments with high(>1000 μM) methane concentration related to the energy of anaerobic methane oxidation. The neogenic labile OM formed during this process is utilized by other groups of microorganisms. According to experimental data, the daily rate of anaerobic methane oxidation is many times higher than that of methanogenesis, which unambiguously indicates the migration nature of the main part of methane.  相似文献   

3.
Lein  A. Yu.  Ivanov  M. V. 《Doklady Earth Sciences》2018,481(1):939-942

The interaction of biogeochemical sulfur and carbon cycles in water bodies has been studied by the different authors and methods, including the use of 35S and 14C radioactive tracers. The main reactions of sulfur and carbon interaction by the example of the Black Sea (sulfate reduction, methanogenesis, aerobic and anaerobic methane oxidation) are considered. Based on the experimental radioisotope data, the annual microbial production of H2S and CH4 in the water column of the Black Sea is estimated. The average annual production of CH4 is 3.8% of the annual production of H2S. The share of migration methane from the bottom sediments (seeps, mud volcanoes, etc.) is approximately 2% of the total dissolved methane pool.

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4.
The stratified water column of the Black Sea is partitioned into oxic, suboxic, and euxinic zones, each characterized by different biogeochemical processes and by distinct microbial communities. In 2003, we collected particulate matter by large volume in situ filtration at the highest resolution to date for lipid biomarker analysis and bacterioplankton for enumeration of major prokaryotic groups. Abundances of several prokaryotic groups were estimated using CARD-FISH probes specific for Bacteria, Archaea (Crenarchaeota and Euryarchaeota), epsilonproteobacteria (mainly sulfide oxidizers) and sulfate reducing bacteria. We also measured a wide range of bacterial and archaeal lipid biomarkers. Depth distributions of diagnostic biomarkers are matched with zonation of microbial processes, including aerobic bacterial oxidation of methane, oxidation of ammonium by bacteria and archaea, metal reduction, and sulfide oxidation at the chemocline, and bacterial sulfate reduction and anaerobic oxidation of methane by archaea in the anoxic zone. Cell densities for archaea and sulfate reducing bacteria are estimated based on water column biomarker concentrations and compared with CARD-FISH results.  相似文献   

5.
南海东北部HD196A岩心的自生条状黃铁矿   总被引：5，自引：0，他引：5       下载免费PDF全文
自生黄铁矿是海洋沉积物缺氧硫酸盐还原过程的主要产物。南海东北部的HD196A岩心中发现大量条状的自生黄铁矿,以中空或实心为主。含量分析表明,岩心500cm附近为黄铁矿富集带,与沉积物有机碳(Corg)、硫酸盐[SO4]2-、甲烷(CH4)以及碳酸钙(CaCO3)的地球化学特征分界一致,是岩心的沉积边界,反映了沉积物所处的缺氧环境。岩心沉积物地球化学剖面表明,有机质参与的硫酸盐还原过程和甲烷厌氧氧化作用是黄铁矿形成的主要因素。黄铁矿异常可以作为指示沉积物甲烷异常的标志之一。  相似文献   

6.
A methane-sulfate coupled reaction diffusion model has been developed to describe the inverse relationship commonly observed between methane and sulfate concentrations in the pore waters of anoxic marine sediments. The sediment column was divided into two zones; an upper zone where diagenetic reaction rates are limited by the concentration of oxidizable organic matter and a lower zone in which reaction rates are limited by the concentration of oxidizing agent—sulfate. For each zone differential equations describing the distribution of methane and sulfate were derived. The boundary conditions used to solve these equations resulted in a set of four coupled equations. When fit to data from Saanich Inlet (B.C., Canada) and Skan Bay (Alaska) the model not only reproduces the observed methane and sulfate pore water concentration profiles but also accurately predicts the methane oxidation and sulfate reduction rates. Maximum methane oxidation rates occur at the transition boundary from the upper to the lower layer. In Saanich Inlet sediments from 23 to 40% of the downward sulfate flux is consumed in methane oxidation while in Skan Bay this value is only about 12%.  相似文献   

7.
A steady-state reaction-transport model is applied to sediments retrieved by gravity core from two stations (S10 and S13) in the Skagerrak to determine the main kinetic and thermodynamic controls on anaerobic oxidation of methane (AOM). The model considers an extended biomass-implicit reaction network for organic carbon degradation, which includes extracellular hydrolysis of macromolecular organic matter, fermentation, sulfate reduction, methanogenesis, AOM, acetogenesis and acetotrophy. Catabolic reaction rates are determined using a modified Monod rate expression that explicitly accounts for limitation by the in situ catabolic energy yields. The fraction of total sulfate reduction due to AOM in the sulfate-methane transition zone (SMTZ) at each site is calculated. The model provides an explanation for the methane tailing phenomenon which is observed here and in other marine sediments, whereby methane diffuses up from the SMTZ to the top of the core without being consumed. The tailing is due to bioenergetic limitation of AOM in the sulfate reduction zone, because the methane concentration is too low to engender favorable thermodynamic drive. AOM is also bioenergetically inhibited below the SMTZ at both sites because of high hydrogen concentrations (∼3-6 nM). The model results imply there is no straightforward relationship between pore water concentrations and the minimum catabolic energy needed to support life because of the highly coupled nature of the reaction network. Best model fits are obtained with a minimum energy for AOM of ∼11 kJ mol−1, which is within the range reported in the literature for anaerobic processes.  相似文献   

8.
Surface sediment samples from the shelf and continental slope off southwest Africa and sediment cores from the deepest part of the Black Sea were analyzed for sterols. Because the organic matter in these anoxic sediments is relatively well-preserved, the input from source organisms in the water column is important in controlling sterol distribution patterns. The sterol distribution on the Namibian shelf is complex, probably because of the great spatial and temporal variability of biological productivity caused by seasonal upwelling and changes in oxygen concentration. The Black Sea, perhaps because of greater physical stability of the water column, has sterol distributions which can be explained by microbial activity or chemical processes acting on a constant input of organic carbon from surface production.  相似文献   

9.
Syngenetic iron sulfides in sediments are formed from dissolved sulfide resulting from sulfate reduction and catabolism of organic matter by anaerobic bacteria. It has been shown that in recent marine sediments deposited below oxygenated waters there is a constant relationship between reduced sulfur and organic carbon which is generally independent of the environment of deposition. Reexamination of data from recent sediments from euxinic marine environments (e.g., the Black Sea) also shows a linear relationship between carbon and sulfur, but the slope is variable and the line intercepts the S axis at a value between 1 and 2 percent S. It is proposed that the positive S intercept is due to watercolumn microbial reduction of sulfate using metabolizable small organic molecules and the sulfide formed is precipitated and accumulates at the sediment-water interface. The variation in slope and intercept of the C to S plots for several cores and for different stratigraphic zones for the Black Sea can be interpreted in relation to thickness of the aqueous sulfide layer or thinness of the oxygen containing layer and to deposition rate, but also may be influenced by availability of iron, and perhaps the type of organic matter (Leventhal, 1979).  相似文献   

10.
The Riogrande II reservoir in Colombia has a total storage capacity of 240 million m3 and lies 2,270 m above sea level. The reservoir is used for power generation, water supply and environmental improvement. Dissolved manganese (Mn) is removed from reservoir water dedicated to domestic use by purification processes. Removal of Mn, however, poses a major challenge to purification processes and warrants the study of ways to naturally reduce dissolved Mn levels in the reservoir. The source of Mn within the reservoir is not well understood, however, presumably arises from sediment mobilization initiated by variation in pH, redox potential (ORP or Eh), dissolved oxygen (O2) and ionic strength conditions. This study investigated conditions within the reservoir to further understand Mn transfer from the sediment into the water column. O2, pH, oxidation–reduction potential (ORP or Eh), organic matter content and electric conductivity were measured in water samples and sediment from the reservoir. Sequential extraction (SE) procedures were used to test the specific effects exerted by each of these conditions on Mn mobilization from the sediments. The European Community Bureau of Reference (BCR) sequential extraction procedure was used to quantify metals in sediment (referred to as the BCR extraction below). Statistical analysis of geochemical data from water samples (both water column and sediment pore water) and sediments demonstrated the conditions under which Mn can be released from sediments into the water column. The results indicated a primarily oxic water column and anoxic reducing conditions in the sediment (ORP or Eh ≤ ?80 mV). The pH of water in contact with bottom sediments varied from 7.6 to 6.8. The pH of sedimentary pore water varied from 6.8 to 4.7. The sediments contained significant amounts of organic matter (20 %). Chemical extractions showed that the exchangeable fraction contained over 50 % of the total Mn within sediments. Microscopic analysis using scanning electron microscopy–energy dispersive spectroscopy (SEM–EDS) indicated that Mn does not occur within well-crystallized mineral phases in the Riogrande II sediments. A large proportion of Mn exists instead as material adsorbed onto the surfaces of recently deposited sediment particles. Bacterial oxidation of organic matter may cause the observed anoxic conditions at the bottom of the reservoir. Mineralization of organic matter therefore contributes to reducing conditions within the sediments. Mobilization of Mn from the sediment into the water column may result from reductive dissolution of this fraction. Manganese release by this mechanism diminishes the water quality of the Riogrande II reservoir and warrants further study.  相似文献   

11.
Partitioning of heavy metals in surface Black Sea sediments   总被引：1，自引：0，他引：1  
Bulk heavy metal (Fe, Mn, Co, Cr, Ni, Cu, Zn and Pb) distributions and their chemical partitioning, together with TOC and carbonate data, were studied in oxic to anoxic surface sediments (0–2 cm) obtained at 18 stations throughout the Black Sea. TOC and carbonate contents, and available hydrographic data, indicate biogenic organic matter produced in shallower waters is transported and buried in the deeper waters of the Black Sea. Bulk metal concentrations measured in the sediments can be related to their geochemical cycles and the geology of the surrounding Black Sea region. Somewhat high Cr and Ni contents in the sediments are interpreted to reflect, in part, the weathering of basic-ultrabasic rocks on the Turkish mainland. Maximum carbonate-free levels of Mn (4347 ppm), Ni (355 ppm) and Co (64 ppm) obtained for sediment from the shallow-water station (102 m) probably result from redox cycling at the socalled ‘Mn pump zone’ where scavenging-precipitation processes of Mn prevail. Chemical partitioning of the heavy metals revealed that Cu, Cr and Fe seem to be significantly bound to the detrital phases whereas carbonate phases tend to hold considerable amounts of Mn and Pb. The sequential extraction procedures used in this study also show that the metals Fe, Co, Ni, Cu, Zn and Pb associated with the ‘oxidizable phases’ are in far greater concentrations than the occurrences of these metals with detrital and carbonate phases. These results are in good agreement with the recent studies on suspended matter and thermodynamic calculations which have revealed that organic compounds and sulfides are the major metal carriers in the anoxic Black Sea basin, whereas Fe-Mn oxyhydroxides can also be important phases of other metals, especially at oxic sites. This study shows that, if used with a suitable combination of the various sequential extraction techniques, metal partitioning can provide important information on the varying geological sources and modes of occurrence and distribution of heavy metals in sediments, as well as, on the physical and chemical conditions prevailing in an anoxic marine environment.  相似文献   

12.
《Applied Geochemistry》1996,11(5):711-720
The organic matter in 9 recent (not more than 250 years old) and ‘organic-rich’ sediments from the southern Black Sea shelf and upper slope have been characterized semi-quantitatively by Pyrolysis/Gas Chromatography/Mass Spectrometry (PY/GC/MS) and13C Cross Polarization Magic Angle Spinning Nuclear Magnetic Resonance (CPMAS-NMR) spectrometry. The organic matter of 7 of the studied sediments was found to be ligno-carbohydrate with a proteinaceous component, one sediment appeared to contain oxidized coal dust and one contained thiophenes in association with pyrite. The ligno component is derived from grasses and soft wood lignin. Material entrapped in an anoxic environment contained the highest proportions of carbohydrate and protein. All the samples had suffered diagenesis as is generally shown by the attachment of carboxyl groups and the removal of methoxyl groups. The evidence suggests that diagenesis occurred whilst the particles traversed the oxic water column.  相似文献   

13.
We evaluate anaerobic oxidation of methane (AOM) in the Black Sea water column by determining distributions of archaea-specific glyceryl dialkyl glyceryl tetraethers (GDGTs) and 13C isotopic compositions of their constituent biphytanes in suspended particulate matter (SPM), sinking particulate matter collected in sediment traps, and surface sediments. We also determined isotopic compositions of fatty acids specific to sulfate-reducing bacteria to test for biomarker and isotopic evidence of a syntrophic relationship between archaea and sulfate-reducing bacteria in carrying out AOM. Bicyclic and tricyclic GDGTs and their constituent 13C-depleted monocyclic and bicyclic biphytanes (down to −67‰) indicative of archaea involved in AOM were present in SPM in the anoxic zone below 700 m depth. In contrast, GDGT-0 and crenarchaeol derived from planktonic crenarchaeota dominated the GDGT distributions in the oxic surface and shallow anoxic waters. Fatty acids indicative of sulfate-reducing bacteria (i.e., iso- and anteiso-C15) were not strongly isotopically depleted (e.g., −32 to −25‰), although anteiso-C15 was 5‰ more depleted in 13C than iso-C15. Our results suggest that either AOM is carried out by archaea independent of sulfate-reducing bacteria or those sulfate-reducing bacteria involved in a syntrophy with methane-oxidizing archaea constitute a small enough fraction of the total sulfate-reducing bacterial community that an isotope depletion in their fatty acids is not readily detected. Sinking particulate material collected in sediment traps and the underlying sediments in the anoxic zone contained the biomarker and isotope signature of upper-water column archaea. AOM-specific GDGTs and 13C-depleted biphytanes characteristic of the SPM in the deep anoxic zone are not incorporated into sinking particles and are not efficiently transported to the sediments. This observation suggests that sediments may not always record AOM in overlying euxinic water columns and helps explain the absence of AOM-derived biomarkers in sediments deposited during past periods of elevated levels of methane in the ocean.  相似文献   

14.
The Dvurechenskii mud volcano (DMV) is located in permanently anoxic waters at 2060 m depth (Sorokin Trough, Black Sea). The DMV was studied during the RV Meteor expedition M72/2 as an example of an active mud volcano system, to investigate the significance of submarine mud volcanism for the methane and sulfide budget of the anoxic Black Sea hydrosphere. Our studies included benthic fluxes of methane and sulfide, as well as the factors controlling transport, consumption and production of both compounds within the sediment. The pie-shaped mud volcano showed temperature anomalies as well as solute and gas fluxes indicating high fluid flow at its summit north of the geographical center. The anaerobic oxidation of methane (AOM) coupled to sulfate reduction (SR) was repressed in this zone due to the upward flow of sulfate-depleted fluids through recently deposited subsurface muds, apparently limiting microbial methanotrophic activity. Consequently, the emission of dissolved methane into the water column was high, with an estimated rate of 0.46 mol m−2 d−1. On the wide plateau and edge of the mud volcano surrounding the summit, fluid flow and total methane flux were lower, allowing higher SR and AOM rates correlated with an increase in sulfate penetration into the sediment. Here, between 50% and 70% of the methane flux (0.07-0.1 mol m−2 d−1) was consumed within the upper 10 cm of the sediment. The overall amount of dissolved methane released from the entire mud volcano structure into the water column was significant with a discharge of 1.3 × 107 mol yr−1. The DMV maintains also high areal rates of methane-fueled sulfide production and emission of on average 0.05 mol m−2 d−1. This is a difference to mud volcanoes in oxic waters, which emit similar amounts of methane, but not sulfide. However, based on a comparison of this and other mud volcanoes of the Black Sea, we conclude that sulfide and methane emission into the hydrosphere from deep-water mud volcanoes does not significantly contribute to the sulfide and methane inventory of the Black Sea.  相似文献   

15.
The reduction of sulfate by sulfate reducing bacteria in the anoxic zone is an extremely important process during early diagenesis of marine sediments. Our data from Great Bay, NH reinforce the proposal that the rate of sulfate reduction is directly proportional to the reactivity of the organic matter or the amount of readily metabolizable organic matter present in the sediment and, hence, the source of the organic material in the anoxic zone. It appears that organic matter rich in marine organic remains is more easily degraded in the anoxic zone and that sulfate reduction rates can vary considerably in an estuarine system where many types of organic material may be deposited.  相似文献   

16.
The redox stratification of bottom sediments in Kandalaksha Bay, White Sea, is characterized by elevated concentrations of Mn (3–5%) and Fe (7.5%) in the uppermost layer, which is two orders of magnitude and one and a half times, respectively, higher than the average concentrations of these elements in the Earth’s crust. The high concentrations of organic matter (Corg = 1–2%) in these sediments cannot maintain (because of its low reaction activity) the sulfate-reducing process (the concentration of sulfide Fe is no higher than 0.6%). The clearest manifestation of diagenesis is the extremely high Mn2+ concentration in the silt water (>500 μM), which causes its flux into the bottom water, oxidation in contact with oxygen, and the synthesis of MnO2 oxyhydroxide enriching the surface layer of the sediments. Such migrations are much less typical of Fe. Upon oxygen exhaustion in the uppermost layer of the sediments, the synthesized oxyhydroxides (MnO2 and FeOOH) serve as oxidizers of organic matter during anaerobic diagenesis. The calculated diffusion-driven Mn flux from the sediments (280 μmM/m2 day) and corresponding amount of forming Mn oxyhydrate as compared to opposite oxygen flux to sediments (1–10 mM/m2 day) indicates that >10% organic matter in the surface layer of the sediments can be oxidized with the participation of MnO2. The roles of other oxidizers of organic matter (FeOOH and SO42−) becomes discernible at deeper levels of the sediments. The detailed calculation of the balance of reducing processes testifies to the higher consumption of organic matter during the diagenesis of surface sediments than it follows from the direct determination of Corg. The most active diagenetic redox processes terminate at depths of 25–50 cm. Layers enriched in Mn at deeper levels are metastable relicts of its surface accumulation and are prone to gradual dissemination  相似文献   

17.
We report solid phase sulfur speciation of six cores from sediments underlying oxic, suboxic and anoxic-sulfidic waters of the Black Sea. Our dataset includes the five sulfur species [pyrite-sulfur, acid volatile sulfides (AVS), zerovalent sulfur (S(0)), organic polysulfides (RSx), humic sulfur] together with reactive iron and manganese, as quantified by dithionite extraction, and total organic carbon. Pyrite – sulfur was the major phase in all cores [200-400 µmol (g dry wt)- 1] except for the suboxic core. However, zerovalent sulfur and humic sulfur also reached very significant levels: up to about 109 and 80 µmol (g dry wt)- 1, respectively. Humic sulfur enrichment was observed in the surface fluff layers of the eastern central basin sediments where Unit-1 type depositional conditions prevail. Elemental sulfur accumulated as a result of porewater sulfide oxidation by reactive iron oxides in turbidities from the anoxic basin margin and western central basin sediments. The accumulation of elemental sulfur to a level close to that of pyrite-S in any part of central Black Sea sediments has never been reported before and our finding indicates deep basin turbidites prevent the build-up of dissolved sulfide in the sediment. This process also contributes to diagenetic pyrite formation whereas in the non-turbiditic parts of the deep basin water column formed (syngenetic) pyrite dominates the sulfur inventory. In slope sediments under suboxic waters, organic sulfur (humic sulfur + organic polysulfides) account for 33-42% of total solid phase S, indicating that the suboxic conditions favor organosulfur formation. Our study shows that the interactions between depositional patterns (Unit 1 vs. turbidite), redox state of overlying waters (oxic-suboxic-sulfidic) and organic matter content determine sulfur speciation and enable the accumulation of elemental sulfur and organic sulfur species close to a level of pyrite-S.  相似文献   

18.
Study of biogeochemical processes in water and sediments of the Chukchi Sea in August 2004 revealed atypical maximums of the concentration of biogenic elements (N, P, and Si) and the rate of microbial sulfate reduction in the surface layer (0–3 cm) of marine sediments. The C: N: P ratio in the organic matter (OM) of this layer does not fit the Redfield-Richards stoichiometric model. Specific features of biogeochemical processes in sea are likely related to the complex dynamics of water, high primary productivity (110–1400 mg C/(m2 day)), low depth of basin (<50 m in 60% of the water area), reduced food chain due to low population of zooplankton, high density of zoobenthos (up to 4230 g m?2), and high activity of microbial processes. Drastic decrease in the concentration of biogenic elements, iodine, total alkalinity (Alk), and population of microorganisms beneath the 0–3 cm layer testify to a large-scale OM decay at the water-seafloor barrier. Our original experimental data support the high annual rate of OM mineralization at the bottom of the Chukchi Sea.  相似文献   

19.
The concentrations of CH4, SO42−, σCO2 and the carbon isotope compositions of ΣCO2 and CH4 in the pore-water of the GS sedimentary core collected from Guishan Island (Pearl River Estuary), South China Sea, were determined. The methane concentration in the pore-water shows dramatic changes and sulfate concentration gradients are linear at the base of the sulfate reduction zone for the station. The carbon isotope of methane becomes heavier at the sulfate-methane transition (SMT) likely because of the Raleigh distillation effect; 12CH4 was oxidized faster than 13CH4, and this caused the enrichment of residual methane δ 13C and δ 13C-ΣCO2 minimum. The geochemical profiles of the pore-water support the existence of anaerobic oxidation of methane (AOM), which is mainly controlled by the quality and quantity of the sedimentary organic matter. As inferred from the index of δ 13C-TOC value and TOC/TN ratio, the organic matter is a mix of mainly refractory terrestrial component plus some labile alga marine-derived in the study area. A large amount of labile organic matter (mainly labile alga marine-derived) is consumed via the process of sedimentary organic matter diagenesis, and this reduces the amount of labile organic matter incorporated into the base of the sulfate reduction zone. Due to the scarcity of labile organic matter, the sulfate will in turn be consumed by its reaction with methane and therefore AOM takes place. Based on a diffussion model, the portion of pore-water sulfate reduction via AOM is 58.6%, and the percentage of ΣCO2 in the pore-water derived from AOM is 41.4%. Thus, AOM plays an important role in the carbon and sulfur cycling in the marine sediments of Pearl River Estuary.  相似文献   

20.
Pyritization in late Pleistocene sediments of the Black Sea is driven by sulfide formed during anaerobic methane oxidation. A sulfidization front is formed by the opposing gradients of sulfide and dissolved iron. The sulfidization processes are controlled by the diffusion flux of sulfide from above and by the solid reactive iron content. Two processes of diffusion-limited pyrite formation were identified. The first process includes pyrite precipitation with the accumulation of iron sulfide precursors with the average chemical composition of FeSn (n = 1.10-1.29), including greigite. Elemental sulfur and polysulfides, formed from H2S by a reductive dissolution of Fe(III)-containing minerals, serve as intermediates to convert iron sulfides into pyrite. In the second process, a “direct” pyrite precipitation occurs through prolonged exposure of iron-containing minerals to dissolved sulfide. Methane-driven sulfate reduction at depth causes a progressive formation of pyrite with a δ34S of up to +15.0‰. The S-isotopic composition of FeS2 evolves due to contributions of different sulfur pools formed at different times. Steady-state model calculations for the advancement of the sulfidization front showed that the process started at the Pleistocene/Holocene transition between 6360 and 11 600 yr BP. Our study highlights the importance of anaerobic methane oxidation in generating and maintaining S-enriched layers in marine sediments and has paleoenvironmental implications.  相似文献   

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