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1.
硫酸盐-甲烷转换带(SMTZ)是海洋富甲烷沉积环境中重要的生物地球化学分带,其内发生的甲烷厌氧氧化反应(AOM)通常能影响多种自生矿物(碳酸盐类、黄铁矿、重晶石和石膏等)的形成过程。本文选取南海东北部天然气水合物赋存区GMGS2-16站位的58个沉积物样品,对其中发育的自生矿物进行了类型、含量、分布、显微形貌和稳定同位素研究。GMGS2-16站位岩心沉积物中主要发育碳酸盐类、黄铁矿和石膏3类自生矿物,亦发现单质硫颗粒的存在。自生矿物含量分布变化较大,存在多个富集层位。自生碳酸盐类均为块状,具极负的δ~(13 )C值(-37.3‰~-51.7‰VPDB)和较重的δ~(18 )O值(3.13‰~4.95‰VPDB),指示其为甲烷碳源,即AOM成因。自生黄铁矿主要呈不规则块状、棒状-管状和生物充填状,δ~(34 )S值变化范围为-41.7‰~27.1‰VCDT,其中δ~(34)S值异常正偏很可能与大量甲烷流体上涌至SMTZ内加强AOM反应有关。多层AOM成因的自生碳酸盐类与δ~(34)S值异常的自生黄铁矿产出层位基本吻合,共同指示了研究站位曾发生过多期次甲烷渗漏事件,可能与研究站位天然气水合物藏失稳存在一定联系。自生石膏主要呈棱柱状和透镜状,偶见黄铁矿-石膏共生体,初步推测自生石膏可能与水合物形成过程中的排离子效应和(或)沉积环境氧化还原条件改变导致的黄铁矿氧化有关。因此,海洋沉积物中碳酸盐类-黄铁矿-石膏自生矿物组合对探讨古海洋甲烷渗漏事件和天然气水合物藏的演化具有重要指示意义。  相似文献   

2.
天然气水合物是一种赋存在低温,高压条件下海底沉积物中的规模巨大的新型能源,研究表明,地球化学是识别海底天然气水合物赋存的一种有效方法。国际上通过分析由大洋钻探采上来的柱状沉积物和孔隙水的地球化学异常,已建立了一套较为成熟的地球化学识别方法。但是,在没有钻井岩心的情况下,如何通过浅表层（＜20m）沉积物和孔隙水及底层海水的地球化学分析来识别海底可能存在的天然气水合物,是国际国内天然气水合物勘查中面临的一道难题,通过对国际上已有数据和资料的全面总结,尝试提出了一系列在海底浅层条件下识别天然气水合物赋存的地球异常标志,包括底层海水的烃类气体及其同位素组成异常,沉积物有机碳和水的含量异常,沉积物中孔隙水的元素和同位素组成异常,沉积物中气体含量异常及沉积物中自生碳酸盐矿物的化学和同位素组成异常等。这些标志的建立将有助于在我国海域开展天然气水合物的勘查工作。  相似文献   

3.
杨玉峰  雷怀彦 《海洋科学》2016,40(8):100-107
对南海北部台西南盆地天然气水合物潜在区(973-4岩芯)碳的形态、含量和稳定同位素组成进行了分析,并探讨了成岩环境因素和细菌种群与碳地球化学行为的关系。结果显示:(1)TOC含量为0.4%~1.3%,δ~(13)CTOC为–26.7‰~–23.9‰,说明973-4岩芯主要为陆源有机质,能够满足微生物产甲烷的需要;DIC和δ~(13)CIC的垂向变异及其显著负相关,指示:973-4岩芯560~890 cm深度段有SO42–驱动的AOM反应。(2)p H、Eh、沉积物粒径等成岩环境参数与TOC、IC、δ~(13)CTOC、δ~(13)CIC等碳地化参数显著相关。(3)细菌种群与DIC、δ~(13)CIC显著相关。结论认为:(1)973-4岩芯碳的地化行为与天然气水合物成藏存在明显响应关系。(2)成岩环境参数的垂向变异与碳的地球化学特征密切相关。(3)细菌种群对碳的地化参数变异有着显著影响。  相似文献   

4.
在天然气水合物发育区海底沉积物中甲烷厌氧氧化作用(AOM)是碳循环的重要组成部分。通过定量计算表层沉积物中甲烷迁移转化通量,可以更准确评估甲烷来源碳对沉积物碳库和海洋深部碳库影响。本文利用反应―运移模型对采集于南海神狐水合物发育区两个站位(SH-W19-PC、SH-W23-PC)采集的孔隙水SO_4~(2-)、溶解无机碳(DIC)、Ca~(2+)剖面进行拟合,同时对DIC碳同位素进行分析,确定近海底沉积物中的碳循环。研究显示两个站位孔隙水中SO_4~(2-)和Ca~(2+)浓度在剖面上随深度呈线性减少,DIC浓度随深度逐渐增加,其δ~(13)C_(DIC)值随深度逐渐降低至约-25‰,表明两个站位存在一定程度的AOM。模拟计算两个站位沉积物孔隙水溶解甲烷向上的通量分别为25.9和18.4 mmol·m~(-2) a~(-1),AOM作用产生的DIC分别占其总DIC量的70.7%和60%。由沉积物向海水中释放的DIC通量占DIC汇的约60%。因此,在天然气水合物发育区向海底渗漏甲烷大部分以DIC的形式进入上覆海水,这些具有极负碳同位素值的甲烷来源的DIC可能对局部深海碳库产生一定的影响。  相似文献   

5.
南海北部东沙海域是典型的水合物成藏区,冷泉活动对其沉积物地球化学特征有显著影响。分析了东沙海域冷泉区973-4站位1 375cm(水深1 666m)和973-5站位935cm(水深2 998m)长的柱状样的总有机碳(TOC)、总硫(TS)含量,并挑选其中的底栖有孔虫进行了碳氧同位素测试。通过沉积物总硫含量分析和临近站位孔隙水数据分析表明,2个站位沉积物均有较浅的硫酸盐甲烷还原界面(SMI)深度和较大的甲烷通量,其中973-4站位硫酸盐甲烷界面深度为海水―沉积物界面以下约900cm,973-5站位硫酸盐甲烷界面深度为海水―沉积物界面以下约750cm。总碳/总硫比值表明冷泉流体活动对沉积物硫埋藏起主导作用。Uvigerina spp.的δ13 C表明末次盛冰期(LGM)之前东沙海域有持续的冷泉活动,而自末次盛冰期以来Uvigerina spp.的δ13 C其偏负程度逐渐变小、冷泉活动逐渐减弱,这可能是海平面上升扩大了天然气水合物稳定区范围,从而抑制了冷泉流体上涌的结果。  相似文献   

6.
硫酸盐-甲烷界面在富甲烷和含天然气水合物的海洋沉积区已经成为一个重要的生物地球化学识别边界.在硫酸盐-甲烷界面之上,沉积物中的硫酸盐因参与分解有机质和甲烷厌氧氧化反应而被消耗,而界面之下沉积物中的甲烷则不断生成,含量逐渐增加.根据该界面附近硫酸盐浓度和甲烷浓度的变化特征,可以判断该区甲烷流体通量的大小,从而指示下伏天然气水合物的可能赋存状况.南海北部陆坡的柱状沉积物孔隙水数据的分析显示,其硫酸盐-甲烷界面埋深比较浅,表明该海域的甲烷通量较高.这种高甲烷通量很可能是由下伏的天然气水合物所引起的,并暗示着该区下伏海底可能有天然气水合物沉积层赋存.  相似文献   

7.
硫酸盐-甲烷界面在富甲烷和含天然气水合物的海洋沉积区已经成为一个重要的生物地球化学识别边界。在硫酸盐-甲烷界面之上,沉积物中的硫酸盐因参与分解有机质和甲烷厌氧氧化反应而被消耗,而其界面之下沉积物中的甲烷则不断生成,含量逐渐增加。根据该界面附近硫酸盐浓度和甲烷浓度的变化特征,可以判断该区甲烷流体通量的大小,从而指示下伏天然气水合物的可能赋存状况。南海北部陆坡的柱状沉积物孔隙水数据的分析显示,硫酸盐-甲烷界面埋深比较浅,表明该海域的甲烷通量较高。这种高甲烷通量很可能是由下伏的天然气水合物所引起的,并暗示着该区下伏海底可能有天然气水合物沉积层赋存。  相似文献   

8.
孟宪伟  张俊  夏鹏  王湘芹 《海洋学报》2013,35(6):190-194
海洋沉积物中的硫酸盐-甲烷反应界面（SMI）的深度变化能够指示下伏甲烷水合物的赋存状态。本文通过对南海北部陆坡天然气水合物潜在分布区沉积物间隙水化学和自生碳酸盐氧、碳同位素组成资料系统分析和对比,探讨了南海北部陆坡沉积物的SMI深度空间变化对下伏甲烷水合物的赋存状态的指示意义。结果表明,南海北部陆坡沉积物的SMI的深度呈现出从西南-东北变浅的趋势,这一趋势与自生碳酸盐的碳同位素组成揭示的甲烷释放量增大趋势有很好的对应关系,进而表明在南海北部陆坡从西南-东北甲烷水合物的埋藏深度变浅或者甲烷水合物的分解程度增大。  相似文献   

9.
实际的天然气水合物明显不同于冷泉碳酸盐岩样品。南海已有诸多冷泉碳酸盐岩的研究,针对具有水合物实际产出的神狐海域沉积物样品开展了GDGTs分析测试研究,试图为其成因、来源、AOM作用、生源等提供信息。研究结果表明:SH7B站位96.5~225.2m的岩心样品中,传统指标总有机碳的δ13 C值和C/N值对南海神狐海域天然气水合物赋存段的沉积物之生源输入指示效果不明显;GDGTs主要以类异戊二烯GDGTs为主,水合物赋存段(155~177m)较非水合物赋存段,支链GDGTs相对百分含量明显增多,类异戊二烯GDGTs相对百分含量明显减少。BIT值进一步明确说明:水合物赋存段比非水合物赋存段,沉积物的陆源有机质输入明显增多。前人研究表明~6 Ma左右南海北部接受了较强的河流碎屑和季风碎屑输入,此次事件造成水合物赋存段(6.0~6.74 Ma)陆源有机质输入增多,结果导致沉积物颗粒粒度增大,孔隙空间增多。较粗颗粒物的大量注入可以改善储层物性,形成上细下粗的有利储集体系,从而为神狐海域天然气水合物提供良好储集空间。  相似文献   

10.
对采自南海北部陆坡东沙海域水合物区HD319、HD196A和GC10站位的浅表层沉积物进行了地球化学特征研究。X射线衍射分析和扫描电镜观察表明,沉积物中存在具有天然气水合物和甲烷渗漏指示意义的自生碳酸盐、硫酸盐和黄铁矿。沉积物孔隙水化学组分分析显示,随着埋藏深度加深,SO42-、Ca2+、Mg2+和Sr2+浓度明显降低,CH4、H2S浓度的增加,以及Mg2+/Ca2+和Sr2+/Ca2+比值急剧增加,与世界上水合物区浅表层沉积物孔隙水中离子浓度异常特征吻合。沉积物顶空气游离烃分析结果和孔隙水化学组分变化,特别是SO42-、H2S和甲烷含量的急剧变化,说明研究区有丰富的气源,赋存水合物的可能性非常大,同时指示了研究区硫酸盐-甲烷界面(SMI)较浅,位于海底之下8m左右。  相似文献   

11.
耦合碳、硫同位素及其它地球化学指征研究海底甲烷渗漏   总被引：1，自引：1，他引：0  
Methane seepage is the signal of the deep hydrocarbon reservoir. The determination of seepage is significant to the exploration of petroleum, gas and gas hydrate. The seepage habits microbial and macrofaunal life which is fueled by the hydrocarbons, the metabolic byproducts facilitate the precipitation of authigenic minerals. The study of methane seepage is also important to understand the oceanographic condition and local ecosystem. The seepage could be active or quiescent at different times. The geophysical surveys and the geochemical determinations reveal the existence of seepage. Among these methods, only geochemical determination could expose message of the dormant seepages. The active seepage demonstrates high porewater methane concentration with rapid SO_4~(2–) depleted, low H_2S and dissolved inorganic carbon(DIC), higher rates of sulfate reduction(SR) and anaerobic oxidation of methane(AOM). The quiescent seepage typically develops authigenic carbonates with specific biomarkers, with extremely depleted ~13C in gas, DIC and carbonates and with enriched ~34S sulfate and depleted ~34S pyrite. The origin of methane, minerals precipitation, the scenario of seepage and the possible method of immigration could be determined by the integration of solutes concentration, mineral composition and isotopic fractionation of carbon, sulfur. Numerical models with the integrated results provide useful insight into the nature and intensity of methane seepage occurring in the sediment and paleooceanographic conditions. Unfortunately, the intensive investigation of a specific area with dormant seep is still limit. Most seepage and modeling studies are site-specific and little attempt has been made to extrapolate the results to larger scales. Further research is thus needed to foster our understanding of the methane seepage.  相似文献   

12.
Authigenic barite nodules associated with modestly 13C-depleted calcium carbonate concretions and 34S-enriched pyrite at the bottom of the Upper Devonian Hanover Shale of western New York provide evidence of sulfate reduction coupled with anaerobic oxidation of methane (AOM). The methane, much of it biogenic in origin, may have diffused upward from Middle Devonian Marcellus Shale and perhaps the Upper Ordovician Utica Shale. Strong 34S enrichment and high δ34S/δ18O values of the barite nodules reflect: (1) substantial kinetic fractionation induced by microbial sulfate reduction perhaps intensified by a low seawater sulfate recharge rate and (2) upward delivery of Ba2+- and CH4- bearing pore fluid sourced within underlying sulfate-depleted deposits. However, the association of authigenic calcium carbonate and barite in the same stratigraphic interval, especially the presence of barite overgrowths on carbonate concretions, is not consistent with what is known of AOM-related mineralization of a sediment column passing downward through the sulfate–methane transition (SMT). The documented early formation of authigenic carbonate followed by barite observed relations may reflect a diminished rate of methanogenesis and/or CH4 supply. The tempered methane flux would have induced the SMT to descend the sediment column enabling barite to form within the same stratigraphic horizon that 13C-depleted calcium carbonate had most recently precipitated. Diminished methane flux may have been caused by burial-related passage of the organic-rich Marcellus Shale below the depth of peak biogenic methane generation and its replacement at that depth interval by organic-lean deposits of the upper part of the Hamilton Group. Subsidence of the SMT would have increased the preservation potential of authigenic barite. However, continued survival of the labile barite as it eventually moved through the SMT suggests that the underlying sulfate-depleted zone was strongly enriched in Ba2+.  相似文献   

13.
The northern slope of the South China Sea is a gas-hydrate-bearing region related to a high deposition rate of organic-rich sediments co-occurring with intense methanogenesis in subseafloor environments.Anaerobic oxidation of methane(AOM) coupled with bacterial sulfate reduction results in the precipitation of solid phase minerals in seepage sediment,including pyrite and gypsum.Abundant aggregates of pyrites and gypsums are observed between the depth of 667 and 850 cm below the seafloor(cmbsf) in the entire core sediment of HS328 from the northern South China Sea.Most pyrites are tubes consisting of framboidal cores and outer crusts.Gypsum aggregates occur as rosettes and spheroids consisting of plates.Some of them grow over pyrite,indicating that gypsum precipitation postdates pyrite formation.The sulfur isotopic values(δ~(34) S) of pyrite vary greatly(from –46.6‰ to –12.3‰ V-CDT) and increase with depth.Thus,the pyrite in the shallow sediments resulted from organoclastic sulfate reduction(OSR) and is influenced by AOM with depth.The relative high abundance and δ~(34) S values of pyrite in sediments at depths from 580 to 810 cmbsf indicate that this interval is the location of a paleo-sulfate methane transition zone(SMTZ).The sulfur isotopic composition of gypsum(from–25‰ to –20.7‰) is much lower than that of the seawater sulfate,indicating the existence of a 34 S-depletion source of sulfur species that most likely are products of the oxidation of pyrites formed in OSR.Pyrite oxidation is controlled by ambient electron acceptors such as MnO_2,iron(Ⅲ) and oxygen driven by the SMTZ location shift to great depths.The δ~(34) S values of gypsum at greater depth are lower than those of the associated pyrite,revealing downward diffusion of 34 S-depleted sulfate from the mixture of oxidation of pyrite derived by OSR and the seawater sulfate.These sulfates also lead to an increase of calcium ions from the dissolution of calcium carbonate mineral,which will be favor to the formation of gypsum.Overall,the mineralogy and sulfur isotopic composition of the pyrite and gypsum suggest variable redox conditions caused by reduced seepage intensities,and the pyrite and gypsum can be a recorder of the intensity evolution of methane seepage.  相似文献   

14.
Authigenic carbonates from outcrops of the northern Apennines consist of small and irregular lenses and exhibit numerous features indicative of cold-seep settings. Detailed petrographic, mineralogical and geochemical studies from two Miocene deposits are presented. The first carbonate outcrop, named Fosso Riconi, is located in the foredeep basin of the Apenninic chain, whereas the second deposit represents a satellite basin called Sarsetta. The stable isotope data from specific carbonate minerals show a wide range of values well known from other palaeoseeps of the Apennine Mountains. The majority of seep carbonates are formed by low-Mg calcite and ankerite. Those minerals have δ13C values between ?7 and ?23‰ V-PDB, suggesting variable amounts of carbonate derived from oxidized methane, seawater (dissolved inorganic carbon) and sedimentary organic matter. Dolomite samples have the lowest δ13C values (?30.8 to ?39.0‰ V-PDB), indicating methane as the main carbon source. The findings suggest an evolutionary formation of the seeps and development of authigenic carbonates influenced by the activity of chemosynthetic organisms, of which large lucinid clams are preserved. Bioirrigation by the clams controlled the sediment–water exchange, and is here considered as an explanation for the anomalous Mg content of the calcite. We hypothesize that the seep carbonates were formed during periods of active methane-rich seepage, whereas during periods of slow seepage carbonate formation was reduced. Despite different geological settings, the two examined deposits of Sarsetta and Fosso Riconi show similar features, suggesting that a common pattern of fluid circulation played a major role in carbonate formation at both seep sites.  相似文献   

15.
Paola Ridge, along the NW Calabrian margin (southern Tyrrhenian Sea), is one of the few reported deep sea sites of precipitation of authigenic carbonates in the Tyrrhenian Sea. Here, the changing composition of the seeping fluids and the dynamic nature of the seepage induced the precipitation of pyrite, siderite and other carbonate phases. The occurrence of this array of authigenic precipitates is thought to be related to fluctuation of the sulfate-methane transition zone (SMTZ).Concretions of authigenic minerals formed in the near sub-bottom sediments of the Paola Ridge were investigated for their geochemical and isotopic composition. These concretions were collected in an area characterized by the presence of two alleged mud volcanoes and three mud diapirs. The mud diapirs are dotted by pockmarks and dissected by normal faults, and are known for having been a site of fluid seepage for at least the past 40 kyrs. Present-day venting activity occurs alongside the two alleged mud volcanoes and is dominated by CO2-rich discharging fluids. This discover led us to question the hypothesis of the mud volcanoes and investigate the origin of the fluids in each different domed structure of the study area.In this study, we used stable isotopes (carbon and oxygen) of carbonates coupled with rare earth element (REE) composition of different carbonate and non-carbonate phases for tracing fluid composition and early diagenesis of authigenic precipitates. The analyses on authigenic precipitates were coupled with chemical investigation of venting gas and sea-water.Authigenic calcite/aragonite concretions, from surficial sediments on diapiric structures, have depleted 13C isotopic composition and slightly positive δ18O values. By contrast, siderite concretions, generally found within the first 6 m of sediments on the alleged mud volcanoes, yielded positive δ13C and δ18O values. The siderite REE pattern shows consistent LREE (light REE) fractionation, MREE (medium REE) enrichment and positive Gd and La anomalies. As shown by the REE distribution, the 13C-depleted composition and their association with chemosymbiotic fauna, calcite/aragonite precipitated at time of moderate to high methane flux close to the seafloor, under the influence of bottom seawater. Authigenic siderite, on the other hand, formed in the subseafloor, during periods of lower gas discharges under prolonged anoxic conditions within sediments in equilibrium with 13C-rich dissolved inorganic carbon (DIC) and 18O-rich water, likely related to methanogenesis and intermittent venting of deep-sourced CO2.  相似文献   

16.
Release of methane from the seafloor throughout the world's oceans and the biogeochemical processes involved may have significant effects on the marine sedimentary environment. Identification of such methane release events in marine sediment records can hence provide a window into the magnitude of ancient seeps. Here, we report on analysis of the geochemical composition of samples in a 12.3 m long sediment core (DH-5) collected from a seep site in the South China Sea (SCS). Our aim has been to investigate whether the evidence for the presence of methane release event within sediments is discernible from solid-phase sediment geochemistry. We show that sedimentary total sulfur (TS), δ34S values of chromium reducible sulfur (δ34SCRS) along with total organic carbon (TOC) and total inorganic carbon (TIC) content can be used to infer the presence of methane release events in cold seep settings. At least three methane release events were identified in the studied core (Unit I at 400–550 cm, Unit II at 740–820 cm, and Unit III at 1000–1150 cm). According to the characteristic of redox-sensitive elements (eg., Mo, U and Mn), we suggest that methane flux has been changed from relatively high (Unit I) to low (Unit II and III) rates. This inference is supported by the coupled occurrence of 34S-enriched sulfides in Unit II and III. AMS 14C dates from planktonic foraminifera in Unit I suggest that high methane flux event occurred at ∼15.4–24.8 kyr BP, which probably resulted in locally-focused aerobic methane oxidation. Overall, our results suggest that TS, TOC, TIC and δ34SCRS have potential for identifying present and fossil methane release events in marine sediments.  相似文献   

17.
Authigenic carbonates from active methane seeps offshore southwest Africa   总被引：2，自引：1，他引：1  
The southwest African continental margin is well known for occurrences of active methane-rich fluid seeps associated with seafloor pockmarks at water depths ranging broadly from the shelf to the deep basins, as well as with high gas flares in the water column, gas hydrate accumulations, diagenetic carbonate crusts and highly diverse benthic faunal communities. During the M76/3a expedition of R/V METEOR in 2008, gravity cores recovered abundant authigenic carbonate concretions from three known pockmark sites—Hydrate Hole, Worm Hole, the Regab pockmark—and two sites newly discovered during that cruise, the so-called Deep Hole and Baboon Cluster. The carbonate concretions were commonly associated with seep-benthic macrofauna and occurred within sediments bearing shallow gas hydrates. This study presents selected results from a comprehensive analysis of the mineralogy and isotope geochemistry of diagenetic carbonates sampled at these five pockmark sites. The oxygen isotope stratigraphy obtained from three cores of 2–5?m length indicates a maximum age of about 60,000–80,000?years for these sediments. The authigenic carbonates comprise mostly magnesian calcite and aragonite, associated occasionally with dolomite. Their very low carbon isotopic compositions (–61.0?<?δ13C ‰ V-PDB?<?–40.1) suggest anaerobic oxidation of methane (AOM) as the main process controlling carbonate precipitation. The oxygen isotopic signatures (+2.4?<?δ18O ‰ V-PDB?<?+6.2) lie within the range in equilibrium under present-day/interglacial to glacial conditions of bottom seawater; alternatively, the most positive δ18O values might reflect the contribution of 18O-rich water from gas hydrate decomposition. The frequent occurrence of diagenetic gypsum crystals suggests that reduced sulphur (hydrogen sulphide, pyrite) from sub-seafloor sediments has been oxidized by oxygenated bottom water. The acidity released during this process can potentially induce the dissolution of carbonate, thereby providing enough Ca2+ ions for pore solutions to reach gypsum saturation; this is thought to be promoted by the bio-irrigation and burrowing activity of benthic fauna. The δ18O–δ13C patterns identified in the authigenic carbonates are interpreted to reflect variations in the rate of AOM during the last glacial–interglacial cycle, in turn controlled by variably strong methane fluxes through the pockmarks. These results complement the conclusions of Kasten et al. in this special issue, based on authigenic barite trends at the Hydrate Hole and Worm Hole pockmarks which were interpreted to reflect spatiotemporal variations in AOM related to subsurface gas hydrate formation–decomposition.  相似文献   

18.
On the passive margin of the Nile deep-sea fan, the active Cheops mud volcano (MV; ca. 1,500 m diameter, ~20–30 m above seafloor, 3,010–3,020 m water depth) comprises a crater lake with hot (up to ca. 42 °C) methane-rich muddy brines in places overflowing down the MV flanks. During the Medeco2 cruise in fall 2007, ROV dives enabled detailed sampling of the brine fluid, bottom lake sediments at ca. 450 m lake depth, sub-surface sediments from the MV flanks, and carbonate crusts at the MV foot. Based on mineralogical, elemental and stable isotope analyses, this study aims at exploring the origin of the brine fluid and the key biogeochemical processes controlling the formation of these deep-sea authigenic carbonates. In addition to their patchy occurrence in crusts outcropping at the seafloor, authigenic carbonates occur as small concretions disseminated within sub-seafloor sediments, as well as in the bottom sediments and muddy brine of the crater lake. Aragonite and Mg-calcite dominate in the carbonate crusts and in sub-seafloor concretions at the MV foot, whereas Mg-calcite, dolomite and ankerite dominate in the muddy brine lake and in sub-seafloor concretions near the crater rim. The carbonate crusts and sub-seafloor concretions at the MV foot precipitated in isotopic equilibrium with bottom seawater temperature; their low δ13C values (–42.6 to –24.5‰) indicate that anaerobic oxidation of methane was the main driver of carbonate precipitation. By contrast, carbonates from the muddy lake brine, bottom lake concretions and crater rim concretions display much higher δ13C (up to –5.2‰) and low δ18O values (down to –2.8‰); this is consistent with their formation in warm fluids of deep origin characterized by 13C-rich CO2 and, as confirmed by independent evidence, slightly higher heavy rare earth element signatures, the main driver of carbonate precipitation being methanogenesis. Moreover, the benthic activity within the seafloor sediment enhances aerobic oxidation of methane and of sulphide that promotes carbonate dissolution and gypsum precipitation. These findings imply that the coupling of carbon and sulphur microbial reactions represents the major link for the transfer of elements and for carbon isotope fractionation between fluids and authigenic minerals. A new challenge awaiting future studies in cold seep environments is to expand this work to oxidized and reduced sulphur authigenic minerals.  相似文献   

19.
南海海槽是潜在的天然气水合物发育区，在表层沉积物中分布有石膏-黄铁矿组合。通过对石膏、黄铁矿的形貌特征、矿物组成、化学元素、硫同位素等的分析，讨论和揭示了石膏-黄铁矿组合的成岩环境、形成机理及其与天然气渗漏的关系。石膏集合体为土块状和多孔状、玫瑰状，表面分布有孔洞或微孔，黄铁矿为莓球状、球粒结块状和虫管状。不同形状的石膏、黄铁矿的化学成分没有明显差别。石膏-黄铁矿的形成机理是海底渗漏的天然气与硫酸盐发生缺氧甲烷氧化反应，产物HS^-与沉积物中的Fe^2＋反应产生FeS并转变为黄铁矿，在形成FeS的过程中产生的H^＋促进碳酸盐溶解，Ca^2＋与SO4^2-达到过饱和沉淀出重。^34S的石膏。因此，石膏-黄铁矿组合是海底存在天然气渗漏的证据，这一发现对开展南沙海槽潜在天然气水舍物的调查以及对天然气渗漏事件的研究具有一定的科学意义。  相似文献   

20.
The geochemical cycling of barium was investigated in sediments of pockmarks of the northern Congo Fan, characterized by surface and subsurface gas hydrates, chemosynthetic fauna, and authigenic carbonates. Two gravity cores retrieved from the so-called Hydrate Hole and Worm Hole pockmarks were examined using high-resolution pore-water and solid-phase analyses. The results indicate that, although gas hydrates in the study area are stable with respect to pressure and temperature, they are and have been subject to dissolution due to methane-undersaturated pore waters. The process significantly driving dissolution is the anaerobic oxidation of methane (AOM) above the shallowest hydrate-bearing sediment layer. It is suggested that episodic seep events temporarily increase the upward flux of methane, and induce hydrate formation close to the sediment surface. AOM establishes at a sediment depth where the upward flux of methane from the uppermost hydrate layer counterbalances the downward flux of seawater sulfate. After seepage ceases, AOM continues to consume methane at the sulfate/methane transition (SMT) above the hydrates, thereby driving the progressive dissolution of the hydrates “from above”. As a result the SMT migrates downward, leaving behind enrichments of authigenic barite and carbonates that typically precipitate at this biogeochemical reaction front. Calculation of the time needed to produce the observed solid-phase barium enrichments above the present-day depths of the SMT served to track the net downward migration of the SMT and to estimate the total time of hydrate dissolution in the recovered sediments. Methane fluxes were higher, and the SMT was located closer to the sediment surface in the past at both sites. Active seepage and hydrate formation are inferred to have occurred only a few thousands of years ago at the Hydrate Hole site. By contrast, AOM-driven hydrate dissolution as a consequence of an overall net decrease in upward methane flux seems to have persisted for a considerably longer time at the Worm Hole site, amounting to a few tens of thousands of years.  相似文献   

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