长江口及其邻近海域孔隙水地球化学特征

对长江口沉积物有机碳、总氮、总磷、Fe、Mn、AI及孔隙水和上覆水体中营养盐、Fe、Mn的含量进行了测试,结合早期成岩模型及地球化学热力学分析,探讨了在河口环境中影响孔隙水营养盐和Fe、Mn分布的主要因素,并对沉积物-水界面营养盐扩散通量进行了估算。结果表明,孔隙水中NH4^＋、NO3^-、PO3^4、H4SiO4和Fe、Mn的含量显著高于上覆水体。早期成岩过程是控制长江口沉积物孔隙水营养盐和Fe、Mn分布的主要因素。NH^4＋剖面暗示长江口近岸和远岸海域存在两类不同的生物地球化学过程。孔隙水Fe、Mn剖面暗示在河口环境中其是有机质降解的重要电子受体。在近岸海域MnO2可能是底部NH4^＋ -N移除的重要机制。长江口孔隙水中低磷酸盐与铁及沉积物中磷的形态有关。通量计算结果显示NH4^＋、NO3^-、PO4^3-、地SiO4、Fe和Mn向上覆水体扩散的通量分别为356—3074μmol／（m2·d）、-45．3～62．6μmol／（m2·d）、-0．3～1．7μmol／（m^2·d）、323—3172μmol／（m^2·d）、3．0～10．5μmol／（m^2·d）和35．7～439．5μmol／（m^2·d）。N、P、Si界面通量对上覆水体浮游生物所需营养盐的贡献分别为0．19％～1．65％、0．13％～0．14％和1．2％～12．2％,因此在考虑长江口区域浮游生物所需营养的来源时,沉积物-水界面营养盐扩散通量可以忽略。     

中国近海沉积物-海水界面化学

《中国近海沉积物—海水界面化学》专著是我国第一部海洋界面化学专著,是著者在其主持的国家自然科学基金项目基础上发表的４０余篇学报级论文的系统总结和精练,专著把海洋中生源物质的循环、生物地球化学过程、颗粒物的垂直沉降通量等,集中体现在沉积物—海水界面这一...     

晚新生代海洋磷循环模拟

理论分析表明,海水磷浓度控制了海洋自生磷沉积和热液磷沉积通量,并以此调节长尺度海洋磷循环的动态平衡.运用质量平衡原理,研究恢复了控制晚新生代海洋磷循环的各种通量,并据此模拟出海水磷浓度的演化.海水磷浓度演化与碳同位素分馏记录的浮游光合生物生长速度的变化一致,揭示在长时间尺度上,浮游光合生物的生长受海水磷含量控制.1500万年以来,大陆风化磷通量急剧增加,致使海洋磷浓度和磷沉积通量增加.海洋磷浓度增加促进了海洋生物生产力,导致海洋大气中生物气溶胶浓度升高,最终通过气溶胶的直接和间接辐射效应驱动晚新生代全球变冷.     

湖泊沉积物-水界面营养元素的生物地球化学作用和环境效应 Ⅰ.界面氮循环及其环境效应

发生在沉积物-水界面的剧烈生物地球化学作用对沉积物和上覆水体具重要的环境效应，然而此方面研究很少。本文通过云贵高原四个湖泊湖水和孔隙水NH和NO剖面，沉积物柱芯不同结合态氮含量剖面分布，界面扩散通量，影响氮循环的因素及它们季节性变化规律等的对比研究，初步揭示了湖泊沉积物一水界面的氮循环及其环境效应。     

东沙海域SMI与甲烷通量的关系及对水合物的指示

硫酸根甲烷界面(SMI)是识别海洋沉积物中天然气水合物赋存(甲烷通量)的一个重要生物地球化学标志.通过对南海北部陆坡东沙海域37个站位浅表层沉积物中孔隙水的SO42-和H2S含量变化和沉积物顶空气甲烷含量的变化等地球化学特性进行分析,研究南海北部东沙海域硫酸根甲烷界面(SMI)的分布情况,通过硫酸根变化梯度估算甲烷通量.研究结果显示,东沙海域存在南部深水区"海洋四号"沉积体和北部浅水区九龙甲烷礁两个水合物有利区域,SMI埋深普遍较浅,指示较高的甲烷通量(3.8×10-3~5.9×10-3 mmol/(cm2·a)),与国际上已发现天然气水合物区的地球化学特征相类似.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,暗示着该区海底之下可能有天然气水合物层赋存.     

南海颗粒物质的通量、组成及其与沉积物积累率的关系初探

通过大孔径时间系列沉积物捕获器的多年测量及对样品的多学科综合分析表明:南海北部与中部深海区1000m左右水深颗粒通量大约为90mg·m-2·d-1,在多数情况下,季风期间的颗粒通量有比较明显的增高。颗粒物主要组成为钙质生物来源的CaCO₃、生物硅、岩源物质及海洋生物来源的有机质。颗粒通量与组成在水柱中的垂向变化表明,生源组分中CaCO₃及有机质随深度具有较为明显的减少。颗粒物侧向运动可能是造成某些时段南海中部深层颗粒通量增加的主要原因。颗粒物质在进入深海沉积物之前,CaCO₃、生物硅均在深层水与沉积物界面之间发生大量的溶解作用。有机质在沉降过程中的减少,一方面是由于硅质与钙质壳体的溶解而使结合在壳体内部的有机质随之溶解造成;另一方面可能与生物及生物地球化学作用有关。岩源物质除水柱沉降之外,还可以通过浊流等底层搬运机制进入南海北部及中部海盆,其中在南海北部这种搬运作用更为明显。     

河口沉积物孔隙水营养盐分布特征及扩散通量

通过2010年夏季在李村河口潮滩区3个站位的采样分析,研究了孔隙水营养盐的分布特征,并利用Fick第一定律估算了沉积物-水界面间营养盐的扩散通量。结果表明,孔隙水营养盐在不同站位间质量浓度不同,呈现出自河口上游向下游逐渐降低的分布趋势。NH₄⁺-N质量浓度为26.21~53.10 mg/L,是孔隙水中营养盐的主要组分。沉积物中有机物的降解反应主要在还原状态下进行,营养盐质量浓度在垂向上的变化受有机质含量及沉积物氧化还原环境改变的综合影响。除NO₃^--N外其他营养盐均由沉积物向上覆水体扩散,沉积物是底层水体营养盐的重要来源。     

全球海水剖面Fe同位素组成的不均一性及其影响因素

全球海水剖面Fe同位素组成存在显著不均一性.对大西洋洋中脊、大西洋近海岸带、东太平洋和西太平洋弧后扩张中心多个站位的海水剖面溶解Fe浓度和Fe同位素组成进行了综合分析,得出以下主要认识:（1）不同区域的海水剖面溶解Fe浓度和Fe同位素组成呈现不同的变化特征,海水Fe同位素的变化趋势与海水溶解氧浓度变化一致,而与海水溶解Fe浓度呈镜像变化关系;（2）不同深度的海水溶解Fe浓度和Fe同位素组成特征的主要控制因素不同.表层海水受到大气降尘、生物作用影响呈现富重Fe同位素特征,受河流的影响Fe同位素组成偏轻;深层海水主要受到深海沉积和海底热液活动的影响,其中沉积物中的非还原溶解Fe导致海水富集重Fe同位素,而受洋中脊热液流体影响的深部海水显著富集轻Fe同位素;（3）将目前已知海底热液溶解Fe通量最小值（0.5 Gmol/a）作为全球大洋的热液溶解Fe通量,利用不同来源的溶解Fe同位素与其通量间的关系估算海底热液对海洋的Fe循环的贡献为~5.5%.由于海底热液流体的Fe通量可能远大于0.5 Gmol/a,因此,海底热液活动对海洋溶解Fe的贡献可能远超过前人的估算结果（6.0%）.      

紫阳黄柏树湾和竹山文峪河毒重石矿床锶同位素及碳氧同位素研究

紫阳黄柏树湾毒重石矿床和竹山文峪河毒重石-重晶石矿床呈层状或似层状产于下寒武统下部或其相当层位的硅质岩中,矿体受岩性和岩相控制作用明显.对矿床中毒重石、钡解石和方解石的锶同位素及碳氧同位素的研究结果表明,形成这些矿物的碳主要来自沉积物中的生物有机质在早期成岩阶段经降解、缩合及脱羧基作用所形成的烃类物质或生物气;而锶主要为沉积物孔隙水中海水锶与沉积物中火山碎屑物质蚀变过程中所释放的锶的混合.毒重石形成于早期成岩阶段沉积物的孔隙水介质中,形成毒重石的成矿流体主要为早期成岩阶段沉积物中由海水、有机质组分和火山物质组分相互叠加和混合而组成的孔隙水有机成矿流体.毒重石矿石中广泛发育的生物碎屑及粒屑结构说明生物作用通过生物成因重晶石 (bio- barite)的形式将海水中的 Ba2 浓集并沉降于海底,形成钡矿床的初始富集体.因而,海水中生物作用和沉积物的早期成岩作用是形成本区毒重石矿床的主要机制.     

湿地沉积物-水界面营养盐交换的定量估算

为有效控制湖泊内源营养盐的释放,探讨了不同物理改良措施(覆沙、底质疏松)对沉积物-水界面营养盐的释放通量控制效果。利用原位孔隙水采样技术(Peeper)来获得沉积物孔隙水剖面,对改良后湿地沉积物孔隙水营养盐的垂向分布及其扩散通量进行了研究。结果发现,改良后沉积含水率、孔隙率分别提高了91%和54%。水土界面附近,随剖面深度增加,孔隙水中PO₄3-、NH₄+、NO₃-及NO₂-浓度分布符合指数关系,PO₄3-、NH₄+在8 cm左右达到最大值。种植芦苇后沉积物孔隙水中PO₄3-、NH₄+均有不同程度的下降,改良措施能有效降低表层弱结合态磷在总磷中比例但增加铁磷的比例,种植芦苇可强化这一效应。运用Fick第一定律对剖面孔隙水营养盐的扩散通量进行估算,发现沉积物经疏松后,NH₄+、PO₄3-的扩散通量由57.47~72.19μg/(m2·d)和2.55~3.21μg/(m2·d)变为-95.54~-130.94μg/(m2·d)和1.50~2.05μg/(m2·d),可考虑疏松沉积物-水界面附近沉积物来作为控制湖泊内源污染的有效手段之一。     

Interstitial water – sediment geochemistry of N, P and Fe and its response to overlying waters of tropical estuaries: a case from the southwest coast of India

 The concentrations of N, P and Fe in surface sediments and interstitial and overlying (bottom and surface) waters of the Ashtamudi estuary located in the southwest coast of India are reported along with the various chemical species of N (NO₂–N, NO₃–N, NH₃–N and total N) and P (organic P, inorganic P and total P) in interstitial and overlying waters and discussed in terms of the physico-chemical environment of the system. The interstitial water exhibits higher salinity values compared to bottom and surface waters, indicating the coupled effects of salt-wedge phenomena and gravitational convection of more saline-denser marine water downward through surface sediments. N, P and Fe as well as their chemical forms are enriched in the interstitial water compared to bottom and surface waters. However, the dissolved oxygen (DO) shows an opposite trend. The marked enrichment of NH₃–N in the interstitial water and its marginal presence in bottom and surface waters, together with the substantial decrease in the DO concentrations of bottom water and consequent increase in the concentrations of NO₂–N and NO₃–N in interstitial and bottom waters, points to the nitrification process operating in the sediment-water interface of the Ashtamudi estuary. The enrichment of total N, P and Fe in the interstitial water compared to the overlying counterparts and the positive correlation of sediment N, P and Fe with mud contents as well as organic carbon indicate that these elements are liberated during the early diagenetic decomposition of organic matter trapped in estuarine muds. Received: 5 Oktober 1998 · Accepted: 9 February 1999     

Benthic fluxes and porewater concentration profiles of dissolved organic carbon in sediments from the North Carolina continental slope

Numerous studies of marine environments show that dissolved organic carbon (DOC) concentrations in sediments are typically tenfold higher than in the overlying water. Large concentration gradients near the sediment–water interface suggest that there may be a significant flux of organic carbon from sediments to the water column. Furthermore, accumulation of DOC in the porewater may influence the burial and preservation of organic matter by promoting geopolymerization and/or adsorption reactions. We measured DOC concentration profiles (for porewater collected by centrifugation and “sipping”) and benthic fluxes (with in situ and shipboard chambers) at two sites on the North Carolina continental slope to better understand the controls on porewater DOC concentrations and quantify sediment–water exchange rates. We also measured a suite of sediment properties (e.g., sediment accumulation and bioturbation rates, organic carbon content, and mineral surface area) that allow us to examine the relationship between porewater DOC concentrations and organic carbon preservation. Sediment depth-distributions of DOC from a downslope transect (300–1000 m water depth) follow a trend consistent with other porewater constituents (ΣCO₂ and SO₄²⁻) and a tracer of modern, fine-grained sediment (fallout Pu), suggesting that DOC levels are regulated by organic matter remineralization. However, remineralization rates appear to be relatively uniform across the sediment transect. A simple diagenetic model illustrates that variations in DOC profiles at this site may be due to differences in the depth of the active remineralization zone, which in turn is largely controlled by the intensity of bioturbation. Comparison of porewater DOC concentrations, organic carbon burial efficiency, and organic matter sorption suggest that DOC levels are not a major factor in promoting organic matter preservation or loading on grain surfaces. The DOC benthic fluxes are difficult to detect, but suggest that only 2% of the dissolved organic carbon escapes remineralization in the sediments by transport across the sediment-water interface.     

Spatial and Temporal Variability of Sediment Organic Matter Recycling in Two Temperate Eutrophicated Estuaries

This paper deals with the spatial and seasonal recycling of organic matter in sediments of two temperate small estuaries (Elorn and Aulne, France). The spatio-temporal distribution of oxygen, nutrient and metal concentrations as well as the organic carbon and nitrogen contents in surficial sediments were determined and diffusive oxygen fluxes were calculated. In order to assess the source of organic carbon (OC) in the two estuaries, the isotopic composition of carbon (δ ¹³C) was also measured. The temporal variation of organic matter recycling was studied during four seasons in order to understand the driving forces of sediment mineralization and storage in these temperate estuaries. Low spatial variability of vertical profiles of oxygen, nutrient, and metal concentrations and diffusive oxygen fluxes were monitored at the station scale (within meters of the exact location) and cross-section scale. We observed diffusive oxygen fluxes around 15 mmol m^?2 day^?1 in the Elorn estuary and 10 mmol m^?2 day^?1 in the Aulne estuary. The outer (marine) stations of the two estuaries displayed similar diffusive O₂ fluxes. Suboxic and anoxic mineralization was large in the sediments from the two estuaries as shown by the rapid removal of very high bottom water concentrations of NO _x ^? (>200 μM) and the large NH₄ ⁺ increase at depth at all stations. OC contents and C/N ratios were high in upstream sediments (11–15 % d.w. and 4–6, respectively) and decreased downstream to values around 2 % d.w. and C/N ≤ 10. δ ¹³C values show that the organic matter has different origins in the two watersheds as exemplified by lower δ ¹³C values in the Aulne watershed. A high increase of δ ¹³C and C/N values was visible in the two estuaries from upstream to downstream indicating a progressive mixing of terrestrial with marine organic matter. The Elorn estuary is influenced by human activities in its watershed (urban area, animal farming) which suggest the input of labile organic matter, whereas the Aulne estuary displays larger river primary production which can be either mineralized in the water column or transferred to the lower estuary, thus leaving a lower mineralization in Aulne than Elorn estuary. This study highlights that (1) meter scale heterogeneity of benthic biogeochemical properties can be low in small and linear macrotidal estuaries, (2) two estuaries that are geographically close can show different pattern of organic matter origin and recycling related to human activities on watersheds, (3) small estuaries can have an important role in recycling and retention of organic matter.     

The lignin geochemistry of marine sediments from the southern Washington coast

Lignin oxidation products and stable carbon isotope distributions are used to investigate the sources, transport, and chemical stability of land-derived organic matter in dated cores of modern sediment from the southern Washington State continental shelf and slope. There is no evidence for significant chemical alteration of lignin compounds in these sediments for time periods of up to 400 yr. Gymnosperm woods and nonwoody angiosperm tissues account for most of the land-derived organic matter in the deposits. These land plant remains have an average δ¹³C of approximately ?25.5% and are concentrated in a narrow band of silty sediment which extends northward from the Columbia River mouth along the mid-shelf. Marine organic matter having an approximate δ¹³C of ?21.5%, strongly predominates in most other shelf and slope environments. Net fluxes of land-derived organic matter into the surface 5 cm of the cores vary directly with sediment accumulation rates. Net fluxes of marine organic material into the surface sediments are highest in environments which favor the preservation of organic matter, but correspond to less than 1% of the primary productivity in the overlying waters.     

Benthic exchange of nutrients in Galveston Bay, Texas

Nutrient regeneration rates were determined at three sites increasing in distance from the Trinity River, the main freshwater input source, to Galveston Bay, Texas, from 1994 through 1996. Diffusive fluxes generally agreed in direction with directly measured benthic fluxes but underestimated the exchange of nutrients across the sediment-water interface. While the fluxes of ammonium and phosphate were directed from the sediment into the overlying waters, the fluxes of silicate and chloride changed in both magnitude and direction in response to changing Trinity River flow conditions. Oxygen fluxes showed benthic production during both summer 1995 and winter 1996, while light-dark deployments showed production-consumption, respectively. Benthic inputs of nutrients were higher at either the middle or outer Trinity Bay regions, most likely due to a higher quality and quantity of the autochthonous organic matter deposited. This feature is consistent with and gives evidence for previously observed non-conservative mixing behaviors reported for nutrients in this region of Galveston Bay. Calculated turnover times, between 7 to 135 d for phosphate, 4 to 56 d for silicate, and 0.3 to 10 d for ammonium were significantly shorter than the average Trinity Bay water residence time of 1.5 yr for the period September 1995 through October 1996. During periods of decreased Trinity River flow and increased residence times, benthic inputs of ammonium and phosphate were 1 to 2 orders of magnitude greater than Trinity River inputs and were the dominant input source of these nutrients to Trinity Bay. The sediments, a sink for silicate when overlying water column concentrations of silicate were elevated, became a source of silicate to the overlying waters of Trinity Bay under reduced flow, high salinity conditions.     

铁元素对海相沉积物早期成岩作用的影响

铁元素是地壳中丰度最高的元素之一,在海相沉积物成岩过程中起着非常重要的作用.铁元素作为海洋初级生产力的微营养元素,影响海相沉积物中有机质的输入,其在早期成岩阶段与硫化物和磷元素的耦合关系,可以促进或者降低有机质的保存;铁元素在海相沉积物早期成岩过程中可以改变孔隙水的化学性质,影响亚稳定碳酸盐矿物的保存,导致碳酸盐沉积物...     

Sediment-water oxygen and nutrient exchanges along the longitudinal axis of Chesapeake Bay: Seasonal patterns,controlling factors and ecological significance

Sediment-water oxygen and nutrient (NH₄ ⁺, NO₃ ^?+NO₂ ^?, DON, PO₄ ^3?, and DSi) fluxes were measured in three distinct regions of Chesapeake Bay at monthly intervals during 1 yr and for portions of several additional years. Examination of these data revealed strong spatial and temporal patterns. Most fluxes were greatest in the central bay (station MB), moderate in the high salinity lower bay (station SB) and reduced in the oligohaline upper bay (station NB). Sediment oxygen consumption (SOC) rates generally increased with increasing temperature until bottom water concentrations of dissolved oxygen (DO) fell below 2.5 mg l^?1, apparently limiting SOC rates. Fluxes of NH₄ ⁺ were elevated at temperatures >15°C and, when coupled with low bottom water DO concentrations (<5 mg l^?1), very large releases (>500 μmol N m^?2 h^?1) were observed. Nitrate + nitrite (NO₃ ^?+NO₂ ^?) exchanges were directed into sediments in areas where bottom water NO₃ ^?+NO₂ ^? concentrations were high (>18 μM N); sediment efflux of NO₃ ^?+NO₂ ^? occurred only in areas where bottom water NO₃ ^?+NO₂ ^? concentrations were relatively low (<11 μM N) and bottom waters well oxygenated. Phosphate fluxes were small except in areas of hypoxic and anoxic bottom waters; in those cases releases were high (50–150 μmol P m^?2 h^?1) but of short duration (2 mo). Dissolved silicate (DSi) fluxes were directed out of the sediments at all stations and appeared to be proportional to primary production in overlying waters. Dissolved organic nitrogen (DON) was released from the sediments at stations NB and SB and taken up by the sediments at station MB in summer months; DON fluxes were either small or noninterpretable during cooler months of the year. It appears that the amount and quality of organic matter reaching the sediments is of primary importance in determining the spatial variability and interannual differences in sediment nutrient fluxes along the axis of the bay. Surficial sediment chlorophyll-a, used as an indicator of labile sediment organic matter, was highly correlated with NH₄ ^?, PO₄ ^3?, and DSi fluxes but only after a temporal lag of about 1 mo was added between deposition events and sediment nutrient releases. Sediment O:N flux ratios indicated that substantial sediment nitrification-denitrification probably occurred at all sites during winter-spring but not summer-fall; N:P flux ratios were high in spring but much less than expected during summer, particularly at hypoxic and anoxic sites. Finally, a comparison of seasonal N and P demand by phytoplankton with sediment nutrient releases indicated that the sediments provide a substantial fraction of nutrients required by phytoplankton in summer, but not winter, especially in the mid bay region.     

Diagenesis of dissolved aluminum in organic-rich estuarine sediments

The sedimentary geochemistry of dissolved Al is complicated by a number of different reactions. In this study we show that complexation by organic matter, adsorption to Fe-oxyhydroxides, and reaction with Si in solution have important effects on the distribution of dissolved Al in sediments. In the absence of physical resuspension of sediment into overlying waters, dissolved Al is rapidly consumed at the sediment-water interface and is subsequently released upon reduction of Fe-oxyhydroxides. This release does not cause noticeable perturbations in dissolved Al concentrations in sediments because of rapid consumption reactions which mask the true mobility of Al. Results suggest that one of the consumption reactions may be due to formation of an Fe-Al-silicate. The amount of authigenic aluminosilicate formed in estuarine sediments must be very small relative to the detrital component. In the deep-sea, however, the long residence time of Fe-oxyhydroxides at the sediment-water interface, with resulting greater accumulation of adsorbed Al may explain the abundance of Al in Fe-smectites reported from many different areas.     

Dissolved aluminium in interstitial waters of recent terrigenous marine sediments from the North Atlantic Ocean

The vertical distribution of dissolved Al in interstitial waters of recent marine sediments has been determined using a fluorimetric analytical method adapted for interstitial water analysis. The results suggest that diagenetic reactions occur in the sediment soon after deposition. A narrow depth zone acting as a source of dissolved Al is found in each core. Outside this zone Al appears to be removed from solution and its concentration decreases to values of 1.5 μgAl/l or less, comparable to those of open ocean waters. Dissolved Al and SiO₂ concentrations in interstitial waters close to the sediment-seawater interface are linearly correlated in most cases, suggesting that the geochemistry of Al may be related to the behaviour of biogenic silica in marine sediments.