大河影响下的边缘海反风化作用

在河口与边缘海区域,大量陆源风化产物的输入和强烈的有机物再矿化作用加速了自生硅酸盐矿物和碳酸盐矿物的生成,这一过程与陆地风化作用相反,被称为反风化作用(Reverse weathering)。反风化作用所导致的自生矿物形成通常在短时间内完成,被认为是平衡大气二氧化碳含量,控制海洋中元素平衡的重要过程。反风化作用的研究方法主要分为直接观察法和化学检测法,前者主要用于自生矿物的结构和元素组成的分析,后者则用于自生铝硅酸盐矿物等定量的研究。反风化作用对海洋环境中碳、硅、常量离子(F~-,Li~+,Na~+,K~+,Ca~(2+)和Mg~(2+)等)和金属元素(Fe,Mn和Al等)等的循环具有重要影响,并促使它们在海洋沉积物中长久埋藏。富含金属氧化物的风化产物的输入,大量易降解有机物和生物硅的沉降,强烈的再矿化作用和次氧/厌氧的成岩条件使得河口与边缘海区域成为反风化作用发生的主要场所。     

海洋沉积物中有机质早期成岩矿化路径及其相对贡献

陆架边缘海沉积物是重要的生物地球化学反应器,海洋中90%以上的有机质沉积于此并在早期成岩作用过程中矿化.其矿化路径包括有氧呼吸、反硝化、锰氧化物还原、铁氧化物还原、SO4(-2)还原和CO2还原,并按生成自由能减少的顺序依次发生,构成理想的氧化还原序列.定量研究有机碳矿化路径及其对有机质矿化的相对贡献对揭示能量分配和碳...     

南海北部神狐水合物赋存区浅表层沉积物自生矿物特征及其成因探讨

通过对南海北部神狐海域Site5B和Site4B站位岩心柱沉积物中自生矿物的类型、形貌特点、丰度和稳定同位素特征的研究,探讨了自生矿物的成因机制。研究表明,沉积物中主要发育黄铁矿和碳酸盐类自生矿物。两个站位中发育的自生矿物的丰度、分布位置、晶体形貌和个体大小等存在明显差异,可能与不同站位中甲烷通量和深部构造有关。自生黄铁矿可能是硫酸盐与甲烷等烃类气体或有机质的厌氧氧化作用的产物,极低负值的硫同位素值可能与硫酸盐还原菌和单质硫歧化菌共同参与有关。自生碳酸盐矿物的成因则相对复杂,其形成过程受多种因素的综合影响。碳同位素值未表现出极低负值,可能是甲烷、有机质和正常海水等碳源混合的结果。     

青海湖的无机碳收支

在全球碳循环中,包括湖泊在内的内陆水体起着十分重要的作用,日益受到关注.面对我国湖泊碳收支状况所知甚少的现状,通过青海湖这一典型湖泊现代溶解无机碳(DIC)输入和沉积物组成的调查和分析,初步评价了青海湖无机碳收支的平衡及其可能控制因素.结果表明,受碳酸盐风化制约,青海湖流域的河水、大气降水和地下水的离子组成均以Ca2+和HCO-3占主导.在占主要贡献的河水中,布哈河(流域最大河流)贡献了其中一半的DIC.与只有约4%左右贡献的地下水相比,大气降水输入了近30%的DIC.近50年来,湖泊沉积物的碳累积速率主要取决于布哈河雨季输入的DIC通量变化.目前处于碳酸盐过饱和的青海湖湖水,将由碳酸盐风化带入湖泊的DIC通过自生碳酸盐沉淀迅速转入沉积物,对大气CO2没有直接的消耗.然而,青海湖湖水的碳并不处在一个稳定的状态,碳酸盐过饱和的湖水则很可能作为大气CO2的源,HCO-3中的碳将随着湖泊水位的下降和温度的升高返回到大气中.     

陆架边缘海环境下金属元素与有机质富集关系探讨

陆架边缘海是“河口—陆架”体系重要的碳汇,黏土矿物作为主要载体将有机质与金属元素吸附于表面或层间,通常表现为粒度、有机质和金属元素含量之间高度正相关。本文通过分析南黄海中部沉积物粒度、总有机碳、主微量元素,探讨三者之间分布特征和相互关系,进一步开展金属元素、有机质与黏土矿物吸附模拟实验,结果表明,酸性条件（pH=4）下适量的金属离子（Zn2+、Ni2+、Pb2+）明显促进伊利石对腐殖酸（有机质主要组成部分）吸附,腐殖酸吸附量达到20.06 mg/g,其中金属离子加入使腐殖酸吸附量提高6.25%;同时碱性条件（pH=8）下金属离子也能够促进伊利石对腐殖酸吸附,腐殖酸吸附量达到15.7 mg/g,金属离子加入使腐殖酸吸附量提高38.9%。金属离子的阳离子键桥作用促进伊利石吸附腐殖酸,且酸性环境下腐殖酸的吸附量高于碱性环境。证实了陆架边缘海背下金属元素的参与对黏土矿物吸附腐殖酸具有明显促进作用,有利于在全球碳循环过程形成边缘海“碳库”,同时海洋酸化可能造成海洋溶解有机质降低和重金属离子浓度升高,对陆架边缘海海洋生态系统平衡构成威胁。     

中国区域碳循环研究进展与展望

中国陆地和海洋生态系统的区域碳循环在全球碳循环过程中占有重要地位。目前,中国陆地生态系统在全球碳循环中的地位和作用已有比较深入的研究,而中国边缘海系统碳循环研究相对薄弱。简要回顾中国碳循环（以现代过程的描述为主）的研究动态,重点阐述中国边缘海碳循环研究概况及CO2的海-气交换、有机碳循环、颗粒有机碳的输出、河流的输运等海洋碳循环过程的关键科学问题。在汇总补充及数据更新的基础上勾画了中国区域碳循环框架。我们认为,中国的区域碳循环过程尚有诸多未知量和不确定性,缺乏把陆、海、气作为一个系统的综合研究,海洋生态系统碳循环研究尤其需要加强。中国边缘海的碳循环研究应当围绕CO2的汇源过程这一碳循环的中心问题,深入开展边缘海碳的生物地球化学及其与大气CO2的耦合作用等方面的研究。     

微生物介导的热融湖碳循环关键过程研究进展

极地超常的变暖引起多年冻土不断退化并形成热融湖,该过程释放温室气体与气候变暖形成正反馈。微生物在碳循环不同环节均发挥着重要作用,理解热融湖中微生物对碳循环的调控机制,对于应对未来气候变化具有重要意义。综述了热融湖微生物参与的关键碳循环过程：梳理了热融湖形成过程和形成后微生物群落组成与分布;对有机碳分解、产甲烷和甲烷氧化等过程中涉及的主要微生物类群进行了总结;凝练了微生物对碳循环的调控机制及受环境变化的影响机制与要素。基于已有研究,得出如下认识：(1)多年冻土融化形成热融湖主要以陆生有机质为主,一些营养物质如磷酸盐、植物纤维素和亮氨酸残基等生物聚合物从陆地进入水体。(2)在多年冻土融化形成热融湖过程中,随着温度和通气条件的改善,有机质及各种生物聚合物可利用性增加了微生物功能基因多样性,提高了微生物对有机碳的分解潜势。温度、底物、溶解氧等和微生物群落的变化引起微生物代谢途径等的改变,从而影响了甲烷产生、甲烷氧化及固碳等过程,最终影响碳循环。(3)为了加深对热融湖中微生物介导碳循环过程的理解,提出了未来研究的方向：借助宏基因组技术及室内培养实验更加清晰地揭示微生物对碳循环各个过程的调节机制,...     

沉积过程对自生黄铁矿硫同位素的约束

自生黄铁矿是海洋沉积物中还原态硫的主要赋存形式,其形成过程与有机质矿化相关,影响全球的C-S-Fe生物地球化学循环。自生黄铁矿硫同位素分馏主要受微生物硫酸盐还原的控制,但近期的研究成果表明局部沉积环境的改变也可以影响黄铁矿硫同位素的组成,特别是在浅海环境。在浅海非稳态沉积环境内,物理再改造和生物扰动作用,导致硫酸盐还原带内生成的硫化物被再氧化,进而影响黄铁矿的硫同位素值。浅海沉积过程容易受到古气候和海平面变化的影响,引起沉积速率的剧烈波动,导致有机质和活性铁输入的不稳定,进而影响成岩系统的开放性和硫酸盐还原速率,最终影响黄铁矿的硫同位素值。另外,沉积速率的改变还影响硫酸盐—甲烷转换带的迁移,造成有机质和甲烷厌氧氧化硫酸盐还原的相互转化,产生不同的硫同位素信号。东海内陆架泥质区为研究沉积过程对自生黄铁矿的形成及其硫同位素组成的约束机制提供了很好的研究材料。该区域有很好的沉积学研究基础,自生黄铁矿丰富、并且个别层位有生物气（甲烷为主）存在,是研究边缘海C-S-Fe循环的理想场所。     

俯冲带中石墨质碳的研究进展

自然界中,石墨质碳可以稳定存在于沉积岩、岩浆岩和变质岩中,由有机质或无机碳酸盐转变而来。随着对俯冲带碳循环研究的不断深入,通常作为副矿物产出在变质岩中的石墨质碳也引起了广泛的关注。相比于碳酸盐矿物和含碳流体,石墨质碳因其低溶解性、低移动性常作为碳汇稳定存在于俯冲带中。然而,在一些特殊的地质条件下(例如流体出现的开放体系中),石墨质碳不再稳定,它会变得活跃并发生迁移。因此,石墨质碳也是俯冲带碳循环研究中的关键载体。本文在综述前人研究成果的基础上,总结了俯冲带中石墨质碳的性质、来源、形成和分解过程,并重点介绍了俯冲带中非生物成因石墨的形成机制、石墨质碳的稳定性以及石墨质碳的释放,全面探讨了石墨质碳在俯冲带碳循环中的重要意义。俯冲带中石墨质碳的成因机制主要有3种:生物有机质石墨化、饱和含碳流体沉淀、碳酸盐矿物的还原反应。俯冲带中石墨质碳可通过分解脱气和溶解的方式释放。俯冲作用和风化侵蚀是石墨质碳全球循环的两个主要过程,其中俯冲作用对石墨质碳的地球内部循环影响较大。     

有机碳—氧化铁结合对海洋环境中沉积有机碳保存的影响

有机碳在海洋环境中的长期保存机制一直是海洋碳循环研究的重点,也是研究气候变化与全球碳循环之间作用和反馈的关键。据估算,表层海洋沉积物中约20%的有机碳是通过与氧化铁的结合而保存下来的,因此与氧化铁结合是有机碳长期保存的关键因素之一。研究表明,有机碳—氧化铁复合物的形成主要通过吸附和共沉淀这2种机制,共沉淀反应是有机碳与氧化铁在海洋环境中结合的主导机制。不同来源的有机物在发生与铁氧化物的共沉淀或吸附作用时是有选择性的,在大部分海洋环境中铁氧化物优先与海洋有机碳结合,但在河口三角洲区域,铁氧化物优先与陆源有机碳结合。大量的陆源输入,较高的初级生产和频繁的再悬浮活动使河口边缘海特别适于开展有机碳—氧化铁结合的相关研究,这也是今后研究的重点方向。     

Sedimentary Organic Carbon Mineralization and Its Contribution to the Marine Carbon Cycle in the Marginal Seas

Continental margin sediments are important ocean carbon repository, and the internal carbon cycle is mainly driven by the mineralization processes of sedimentary organic matter. Most organic carbon is transformed to Dissolved Inorganic Carbon (DIC) by mineralization processes after being delivered to continental margin sediments, and DIC from pore water diffuses into the upper water column and participates in the ocean carbon cycle. At the same time, some DIC combines ions such as Ca²⁺ and Mg²⁺ and precipitates as authigenic carbonate minerals so that carbon is stored in the deposits. Based on the biogeochemical study of the mechanism and efficiency of organic matter burial, we discussed the interaction among sulfate reduction, methanogenesis and anaerobic oxidation of methane, and the effect of organic mineralization on the formation of authigenic carbonate. By reviewing the above-mentioned aspects, we can obtain a better understanding of the role of continental margin sediments in the global carbon cycling budgets as well as its climate and environmental effects.     

扬子克拉通古大陆边缘Mo同位素特征及对有机埋藏量的指示意义

通过对扬子克拉通古大陆边缘不同时期沉积岩的Mo同位素进行测定,结合Mo微量元素组成,对古大陆边缘Mo的自生作用规律进行了研究,并根据Mo丰度对原始有机碳堆积速率进行了计算.结果表明,其原始有机碳堆积速率在0.17～0.67mmol/m2/day之间.利用已建立的现代大陆边缘δ98Mo与有机碳埋藏速率模型,对该区不同时期沉积岩的有机碳埋藏速率进行恢复.结果表明,扬子克拉通显生宙不同时期沉积岩的有机碳埋藏速率有较大的变化范围(0.43～2.87mmol/m2/day),并与原始有机碳堆积速率具有明显的相关性,因此,δ98Mo有可能成为评价有效烃源岩的潜在指标.     

Authigenic carbonate burial in the Late Devonian–Early Mississippian Bakken Formation (Williston Basin,USA)

Late Devonian (Famennian) marine successions globally are typified by organic-rich black shales deposited in anoxic and euxinic waters and the cessation of shelf carbonate sedimentation. This global ‘carbonate crisis’, known as the Hangenberg Event, coincides with a major extinction of reef-building metazoans and perturbations to the global carbon cycle, evidenced by positive carbon-isotope excursions of up to 4‰. It has been suggested that authigenic carbonate, formed as cements in sedimentary pore spaces during early burial diagenesis, is a significant mass fraction of the total global carbon burial flux, particularly during periods of low oxygen concentration. Because some authigenic carbonate could have originated from remineralization of organic carbon in sediments, it is possible for this reservoir to be isotopically depleted and thereby drive changes in the carbon isotopic composition of seawater. This study presents bulk isotopic and elemental analyses from fine-grained siliciclastics of the Late Devonian–Early Mississippian Bakken Formation (Williston Basin, USA) to assess the volume and isotopic composition of carbonates in these sediments. Carbonate in the Bakken black shales occurs primarily as microscopic disseminated dolomite rhombs and calcite cements that, together, comprise a significant mass-fraction (ca 9%). The elemental composition of the shales is indicative of a dynamic anoxic to sulphidic palaeoenvironment, likely supported by a fluctuating chemocline. Despite forming in an environment favourable to remineralization of organic matter and the precipitation of isotopically depleted authigenic carbonates, the majority of carbon isotope measurements of disseminated carbonate fall between −3‰ and +3‰, with systematically more depleted carbonates in the deeper-water portions of the basin. Thus, although there is evidence for a significant total mass-fraction of carbonate with contribution from remineralized organic matter, Bakken authigenic carbonates suggest that Famennian black shales are unlikely to be sufficiently ¹³C-depleted relative to water column dissolved inorganic carbon to serve as a major lever on seawater isotopic composition.     

Enriched stable carbon isotopes in the pore waters of carbonate sediments dominated by seagrasses: Evidence for coupled carbonate dissolution and reprecipitation

Studies of the δ¹³C of pore water dissolved inorganic carbon (δ¹³C-DIC) were carried out in shallow water carbonate sediments of the Great Bahamas Bank (GBB) to further examine sediment-seagrass relationships and to more quantitatively describe the couplings between organic matter remineralization and sediment carbonate diagenesis. At all sites studied δ¹³C-DIC provided evidence for the dissolution of sediment carbonate mediated by metabolic CO₂ (i.e., CO₂ produced during sediment organic matter remineralization); these observations are also consistent with pore water profiles of alkalinity, total DIC and Ca²⁺ at these sites. In bare oolitic sands, isotope mass balance further indicates that the sediment organic matter undergoing remineralization is a mixture of water column detritus and seagrass material; in sediments with intermediate seagrass densities, seagrass derived material appears to be the predominant source of organic matter undergoing remineralization. However, in sediments with high seagrass densities, the pore water δ¹³C-DIC data cannot be simply explained by dissolution of sediment carbonate mediated by metabolic CO₂, regardless of the organic matter type. Rather, these results suggest that dissolution of metastable carbonate phases occurs in conjunction with reprecipitation of more stable carbonate phases. Simple closed system calculations support this suggestion, and are broadly consistent with results from more eutrophic Florida Bay sediments, where evidence of this type of carbonate dissolution/reprecipitation has also been observed. In conjunction with our previous work in the Bahamas, these observations provide further evidence for the important role that seagrasses play in mediating early diagenetic processes in tropical shallow water carbonate sediments. At the same time, when these results are compared with results from other terrigenous coastal sediments, as well as supralysoclinal carbonate-rich deep-sea sediments, they suggest that carbonate dissolution/reprecipitation may be more important than previously thought, in general, in the early diagenesis of marine sediments.     

Preservation of particulate non-lithogenic uranium in marine sediments

Particulate non-lithogenic uranium (PNU), excess U above detrital background levels found in marine particulate matter, is formed in surface waters throughout the ocean. Previous studies have shown that PNU is regenerated completely prior to burial of particles in sediments within well-oxygenated open-ocean regions. However, the fate of PNU has never been examined in ocean margin regions or in anoxic basins. Here we evaluate the preservation of PNU in ocean margin sediments and within semi-enclosed basins using samples from sediment traps deployed at multiple depths and surface sediments. Organic carbon fluxes at the sediment trap locations ranged from 0.1 to 4.3 g/cm² kyr, while the dissolved oxygen concentration in the water column ranged from <3 μM to ∼ 270 μM. Preservation of PNU increases with decreasing dissolved oxygen concentration, approaching 100% preservation at oxygen concentration < 25 μM. PNU contributes as much as 40 to 70% of the total authigenic U in sediments in the Santa Barbara Basin and seasonally anoxic Saanich Inlet, and some 10% to 50% of the total authigenic U in sediments off the central California Margin.     

Origin of glauconite in the recent bottom sediments of the ocean

There are two general types of sedimentary glauconite in Recent ocean sediments: terrigenous-allogenic and authigenic glauconite. Recent sediments of the oceans contain mainly terrigenous-allogenic glauconite (shelf and continental slope) which is formed from ancient glauconite-bearing rocks on coasts, islands and the ocean floor. The age of terrigenous-allogenic glauconite ranges from 2 to 70 m.y. (8 samples from the Atlantic Ocean, 13 from the Pacific Ocean, 1 from the Indian Ocean). The area of terrigenous-allogenic glauconite distribution correlates very well with the area of distribution of glauconite-bearing rocks on land and does not correlate with the climate and bathymetry.Authigenic glauconite is seldom found in Recent ocean sediments. The sediments with authigenic glauconite form transition zones between sediments with organic carbon, H₂S and sulphide near coasts and oxidized sediments of the ocean floor (red clay and others). The areas of authigenic glauconite distribution are not yet well known. The formation of authigenic glauconite occurs mainly during diagenesis of sediments by synthesis from interstitial solutions and/or alteration of clay minerals.     

水库现代沉积过程沉积磷的早期成岩作用模型研究

在沉积磷形态分析、孔隙水化学、核素计年以及吸附解吸实验等的基础上,运用一维“反应-平流-扩散”模型,研究了红枫湖现代沉积过程中磷的沉积改造。结果表明:红枫湖现代沉积过程中,有机态磷的矿化分解和铁结合态磷的络合/溶解,是控制沉积物磷迁移转化动力学的主要机制。沉积物-水界面附近有机磷的快速降解,可能克服沉积界面上铁氧化物对溶解磷的吸附缓冲,而形成向水体的磷酸盐迁移通量;自生磷灰石的沉积改造相对不明显,沉积磷向稳定形态含磷矿物(钙氟磷灰石)的转化过程同样不能影响红枫湖现代沉积过程中磷转化的质量平衡。     

Authigenic uranium: Relationship to oxygen penetration depth and organic carbon rain

We have measured U in benthic incubation chambers, sediment pore waters, and in sediments along the California continental margin. Sedimentary U uptake rates, based on a combination of sediment pore water profiles and benthic incubation chambers, generally agree with those predicted from sediment accumulation rate data. This agreement supports the view that most of the continental margin sedimentary U is delivered by diffusion across the seawater-sediment boundary. The average rate of authigenic U accumulation for all the sites examined here is ∼−0.2 nmol cm^-2 y^-1, which is consistent with published global estimates of sedimentary U uptake. In addition, the accumulation rate of U in sediments exhibits a nonlinear relationship with the oxygen penetration depth and a linear relationship with the organic carbon rain rate. These relationships highlight the potential utility for the U accumulation rate as a proxy for these processes.     

Role of a strong oxygen-deficient zone in the preservation and degradation of organic matter: a carbon budget for the continental margins of northwest Mexico and Washington State

Rates of organic carbon oxidation in marine sediments were determined for the continental margins of northwest Mexico and Washington State, with the goal of assessing the role of oxygen in the preservation of organic matter on a margin with a strong oxygen-deficient zone and on a typical western continental margin. Total carbon oxidation rates (including rates for individual electron acceptors: O₂, NO₃⁻, and SO₄⁼) were determined at depths ranging from 100 to 3000 m on both margins. Carbon oxidation rates were generally higher on the Washington margin than on the Mexican margin. The relative importance of the different electron acceptors varied across the two margins and was related primarily to the availability of O₂ and NO₃⁻ from the overlying water. The relative contribution of O₂ consumption increased in deeper sediments (>2000 m) as aerobic processes began to dominate the total carbon oxidation rate. Denitrification rates were highest in Washington sediments; however, denitrification represented a larger fraction of the total carbon oxidation rate in the Mexican sediments (∼40% for Mexico vs. ∼30% for Washington). Sulfate reduction accounted for as much as 79% of the total carbon oxidation rate in shallow sediments and less than 20% in deep sediments on both margins. The offshore trends in carbon oxidation rate appeared to be related to the organic carbon input rate. Pore-water O₂ and NO₃⁻ penetration depths were shallowest in nearshore stations and increased offshore. Regeneration ratios of C:N:P reveal “non-Redfield” behavior on both margins. Carbon budgets for the two margins demonstrate that off Mexico, a much greater percentage of the organic matter produced in the surface ocean reached the sediments (>15% vs. <8% for Mexico and Washington, respectively). On the Mexican margin, ∼8% of the primary production escaped oxidation in the surface sediments to be permanently buried, as compared with only ∼1.2% of the primary production on the Washington margin. This suggests that oxygen-deficient conditions on Mexican margin are linked to enhanced carbon preservation.     

利用稳定同位素技术研究广西桂江流域水体中碳的来源

本文对岩溶区不同类型样品中的有机碳同位素样品前处理的分离提纯技术进行了研究,并对广西桂江流域水体进行了稳定有机碳同位素分析.结果表明,C3植物对桂江水体可溶性有机碳(DOC)有很大比例的贡献,而水生生物对水体有机碳影响较小.抚河流域比漓江流域有较高的(DOC)含量,可能与非岩溶区土壤微生物活动强,土壤活性有机碳含量高有...