贵阳市阿哈湖水体和沉积物间隙水中汞的含量和形态分布初步研究

为了弄清楚酸性矿井废水的排放是否对阿哈湖造成了汞污染,我们研究了阿哈湖中汞的各种赋存形态(包括溶解气态汞、活性汞、颗粒态汞、溶解态汞、溶解态甲基汞、颗粒态甲基汞,以及沉积物间隙水体的溶解态汞和溶解态甲基汞)及其在水体和沉积物间隙水中的剖面分布.实验数据表明,溶解态甲基汞浓度在沉积物下2～5 cm处最高,随深度增加而逐渐降低,与硫酸盐还原菌(SRB)的分布相吻合,说明水体-沉积物界面是甲基汞的产生地点;并且在沉积物中高浓度硫酸根浓度高达1100mg/L时,硫酸根浓度与甲基汞浓度依然一致.     

沉积物-水界面的生物地球化学作用

沉积物－水界面是天然水体在物理、化学和生物特征等方面差异性最显著和负责水体和沉积物之间物质输送和交换的重要边界环境。对沉积物－水界面生物地球化学的定义、研究方法和它在水体微量物质循环中所起的作用、物质迁移方式、典型氧化还原敏感性元素转化反应（Ｃ、Ｏ、Ｎ）、界面扩散通量和表面扩散亚层的意义和估算等进行了讨论。      

海洋沉积物孔隙水硫酸盐的硫、氧同位素组成及其对硫生物地球化学过程的指示

海洋沉积物中由微生物硫酸盐还原作用(MSR)驱动的碳、硫耦合作用及甲烷消耗,是影响全球碳、硫循环和气候变化的关键生物地球化学过程。准确认识微生物硫酸盐还原代谢过程及其环境影响因子,是探究MSR驱动的碳、硫循环及生态环境效应的重要基础。沉积物孔隙水中硫酸盐的硫、氧同位素组成是揭示MSR过程及其驱动的硫循环的重要方法。本文从细胞内代谢途径和胞外硫循环过程角度,厘清影响孔隙水硫酸盐硫、氧同位素组成的硫的生物地球化学过程,阐述其在示踪有机质驱动和甲烷驱动的硫酸盐还原过程类型及“隐秘”硫循环的意义,为探究微生物硫酸盐还原作用在地球表层环境演化中的作用提供新启示。     

贵阳地区雨水化学与Sr同位素地球化学

贵州省属全国酸雨重灾区之一,尤其以贵阳市更为严重。酸雨会产生一系列不利影响,诸如森林、草地衰亡,土壤酸化板结使农作物减产,引起土地荒漠化等。对酸雨中物质来源的正确认识是评价酸雨和大气环境质量的基础。一般地,雨水中的溶解物质可以分为3部分:1)来源于海盐气溶胶;2)来源于陆地气溶胶(土壤尘埃等);3)来源于人为活动(工业、农业、植被和石化燃料的燃烧及化肥的施用等)。通常区分出雨水中溶质的不同来源是很困难的,同位素方法却有助于雨水源区物质的识别。     

硫酸盐还原菌及异化铁还原菌对 黄钾铁矾还原作用的对比

选取酸性矿坑水环境中常见的次生含铁硫酸盐矿物———黄钾铁矾[KFe3(SO4)2(OH)6]为研究对象,用硫酸盐还原菌 Desulfovibriovulgaris 和异化铁还原菌Shewanellaputrefaciens CN32对其进行还原实验,探讨作为重金属治理潜在材料的 黄钾铁矾的微生物稳定性.实验采用非增长型培养基,在中性、厌氧、30℃的条件下进行.采用湿化学方法测量水溶液及还原产 生的总Fe2+ ,利用X射线衍射(X-raydiffraction,简称XRD)来分析反应后残余固体物质的矿物组成,用扫描电镜(scanning electronicmicroscopy,简称SEM)观察固体残余物的形貌特征.结果表明,没有微生物的参与,黄钾铁矾的稳定性较好.异化铁 还原菌S.putrefaciens CN32和硫酸还原菌D .vulgaris 在营养极其匮乏的中性厌氧条件下均能还原黄钾铁矾晶格中的 Fe3+ ,显示出黄钾铁矾被微生物还原的可能性.S.putrefaciens CN32还原黄钾铁矾晶格中Fe3+ 的最大还原速率和最终Fe3+ 还原率分别为0.001mmol·L-1·h-1和0.37%.与S.putrefaciens CN32不同,D .vulgaris 对黄钾铁矾的还原能力较强,不 含有电子穿梭体(Anthraquinone-2,6-disulfonate,简称AQDS)的实验体系中Fe3+ 的最大还原速率和最终Fe3+ 还原率分别为 0.017mmol·L-1·h-1和16.80%,而添加了AQDS的实验体系的则分别达到了0.026mmol·L-1·h-1和24.30%,这可能与 黄钾铁矾中含有SO42- 有关.D .vulgaris 优先还原黄钾铁矾晶格中的SO42- 产生的H2S是强还原剂,也可促进Fe3+ 的还原, 微生物以及H2S的双重作用可能是导致D .vulgaris 体系中Fe3+ 还原率较高的原因.XRD分析表明,黄钾铁矾经过S.putrefaciens CN32的作用,物相没有发生变化;而经过D .vulgaris 作用后,黄钾铁矾的特征峰消失,固相残余物中出现了菱铁 矿(FeCO3)、蓝铁矿[Fe3(PO4)2·8H2O]等次生矿物.由于培养基中没有添加任何的磷酸盐,因此蓝铁矿的出现可能是由于培 养基中添加的少量酵母浸膏降解后产生的磷酸根与D .vulgaris 还原黄钾铁矾产生的Fe2+ 相互作用的结果.这些认识对深入 理解地球表层铁的生物地球化学循环具有重要意义,为矿山环境重金属的污染治理提供了实验依据.      

长江口沉积物-水界面砷的迁移转化机制与微生物调控分析

为探析长江口沉积物-水界面砷的迁移转化机制,本文分析了2019年夏季长江口4个站位上覆水和间隙水中总As浓度及形态的剖面变化特征,耦合氧化还原敏感元素(Fe、Mn和S)的剖面变化剖析了沉积物-水界面砷循环的Fe-Mn-S控制机制,同时结合砷相关功能基因探讨了沉积物-水界面砷迁移转化的微生物调控过程,估算了沉积物-水界面总As的扩散通量。结果表明,除A7-4站位外,长江口其他3个站位间隙水总As以As³⁺为主要存在形态,且总As浓度均在上覆水中为最低值(0.748~1.57 μg·L^-1),而在间隙水中随着深度增加而逐渐增加并在6~9 cm深度达到峰值(7.14~26.9 μg·L^-1)。间隙水总As及As³⁺浓度的剖面变化趋势与溶解态Fe²⁺、Mn²⁺相似,其均在中间层出现高值,说明沉积物Fe/Mn还原带砷的释放可能是随固相Fe(Ⅲ)或Mn(Ⅳ)的还原而转移到间隙水中的。氧化层和Fe/Mn还原带过渡区间隙水砷浓度与砷异化还原菌功能基因arrA和arsC丰度存在对应关系(除A1-3站外),说明砷异化还原菌将溶解As⁵⁺或固相As⁵⁺还原为溶解As³⁺可能是该过渡层砷迁移转化的另一重要过程。硫酸盐还原带的间隙水总As和As³⁺浓度降低,但由于间隙水的低S^2-浓度不利于砷硫化物生成,因此深层间隙水砷可能与铁硫矿物结合而被移除。底层环境氧化还原条件是影响沉积物-水界面砷迁移转化的重要因素,随底层水DO浓度的降低,砷迁移转化更倾向于微生物还原控制。长江口沉积物-水界面总As的扩散通量为1.18×10^-7~2.07×10^-7 μmol·cm^-2·s^-1,均表现为沉积物间隙水中总As向上覆水释放,即沉积物是研究区域水体总As的来源之一。     

现代湖泊沉积有机氮同位素与废水氮输入演化

湖泊沉积有机氮同位素组成与有机质的来源有关。     

泥河湾盆地第四系有孔虫化石群锶同位素及其古环境意义

泥河湾组含有孔虫化石层位的沉积环境问题存在很大争议。本文从生物壳体的锶同位素地球化学特征对其中的有孔虫进行了进一步研究。样品采自泥河湾小渡口剖面27,28层的有孔虫化石(NonionshansiensisWang)和与其共生的介形虫和腹足类。同时,对该剖面22层介形虫以及流经该剖面的桑干河和支流壶流河河水的87Sr／86Sr值也进行了测定。     

农林生态系统的转变对土壤有机质影响的C示踪研究

生态转变系统中土壤有机质的变化与土壤的初级生产力和温室气体的释放有着密切的关系。同时 ,它也是目前农业的可持续发展和全球环境变化的研究内容之一。对于毁林造田和退耕还林等农林生态系统发生转变的特殊地点 ,土壤有机质的源物质产生了Ｃ3植物 (森林 )与Ｃ4 植物 (农作物 )的转变 ,这就为我们利用δ13Ｃ来示踪土壤有机质的迁移和赋存提供了可能。茂兰保护区曾长期生长Ｃ3植物 (常绿混叶林 ) ,近几十年 ,部分毁林后种植Ｃ4 植物 (玉米 )。本实验分别采集 3个剖面相邻的森林点和农田点的土壤样品 ,分析了样品的有机碳含量和δ13Ｃ值。     

云贵高原湖泊CO2的地球化学变化及其大气CO2源汇效应

湖泊是大气CO₂的源还是汇,长期以来一直都存有争议。云贵高原地区的湖泊由于受流域碳酸盐岩风化作用的影响,使这一问题就显得更特殊,也更复杂。本次研究通过化学平衡计算和气相色谱测定两种方法得到了比较一致的湖水CO₂浓度结果。研究发现,在夏季强烈的光合作用消耗了湖水CO₂,致使湖水中CO₂浓度降低。在贵州草海、百花湖以及云南的泸沽湖、杞麓湖,表层湖水CO₂分压(为便于与大气CO₂比较,文中湖水CO2用分压单位表示)小于200μatm,远低于大气CO₂分压,湖泊正不断地从大气中吸收CO₂,从而构成大气CO₂的汇。     

Seasonal variations of adsorption/desorption equilibrium concentrations of P at water-sediment interface in the Meiliang Bay, Taihu Lake, China

Seasonal variations of adsorption/desorption equilibrium were investigated by collecting overlying water and seasonal sediment from the Meiliang Bay, Taihu Lake, China. At the same time, seasonal variations of TP and P fractions＇ concentrations in the initial and end of adsorption experiment were also carried out. In addition, the effects of temperature on the P translocation process were also conducted and discussed. The following conclusions were obtained： The sequence of adsorption/desorption equilibrium concentrations of P at water-sediment interface was spring〈winter〈autumn. In sediment the concentrations of TP decline. Concentration P decreased with temperature.     

Seasonal variations of adsorption/desorption equilibrium concentrations of P at water-sediment interface in different trophic states of Taihu Lake, China

Sediment from three different trophic states （Meiliang Bay, Xukou Bay and Gonghu Bay） in spring, summer, autumn and winter were collected and analyzed in Taihu Lake. At the same time, seasonal variations in adsorption/desorption equilibrium were investigated with corresponding sediments from these three trophic states, including adsorption efficiency, adsorption/desorption equilibrium concentration and equilibrium adsorption quantity. Variations of TP and P fractions＇ concentrations in the initial and end of adsorption experiment were also documented in order to find the most active P fractions. The following conclusions were obtained： （1） Concentrations of total phosphorus （TP） and its fractions in the sediments were coincided with the trophic state of corresponding overlying water, Meiliang Bay〉Gonghu Bay〉Xukou Bay. The Meiliang Bay located in the north of Taihu Lake is in the eutrophic state and belong to alga-type lake; the Xukou Bay located in the northeast of Taihu Lake is relatively clean lake region; the Gonghu Bay is located in the east of Taihu Lake is in the meso-trophic state. Fe-P concentrations in the Meiliang Bay, Gonghu By and Xukou Bay account for 35.1%-70.9%, 19.6%-26.8%, 16.5%-34.3% of TP, Ca-P account for 20.6%-43.7%, 40.7%-45.0%, 23.0%-41.1% and OP accounts for 15.3%-20.2%, 28.4%-37.4%, 23.6%-54.3%, which changes obviously in different seasons. Fe-P is the major fraction in the eutrophic lake region, which is significantly correlated with the TP concentrations. （2） Adsorption and desorption processes in these three lake regions varied with season.     

Jurassic kimberlites from Picton and Varty Lake,Ontario: Geochemical and stable isotopic characteristics

Micaceous ultramafic dikes of Jurassic age from Picton and Varty Lake, Ontario, consist mineralogically of olivine — phlogopite — serpentine — calcite-spinel. The rocks are characterized by abundant Ba-rich phlogopite (up to 6.5 wt.% BaO) and spinels with a diagnostic kimberlite trend-1. Compositionally the dikes are characterized by extreme silica-undersaturation (21–30 wt.% SiO₂), primitive Mg/(Mg + Fe^T) ratios (0.75–0.83), large enrichments of volatile components (CO₂ and H₂O), and relatively high abundances of both incompatible and compatible trace elements. The dikes exhibit pronounced enrichments of light rare earth elements (LREE) (La_N=320–1330) combined with strongly fractionated patterns (La_N/Yb_N=45–108). Calcite in the dikes is a primary magmatic phase, from textural relations and C-isotopic compositions ( ¹³C= –4.0 to –8.3). A calcite-rich aphanitic phase of the Picton dike is interpreted to be a late stage magmatic differentiate, which possibly involved olivine fractionation. Although the dikes lack most of the macrocrysts generally considered to be important diagnostic minerals of kimberlite magmatism, the geochemical, mineralogical and C- and O-isotopic characteristics collectively indicate that the dikes are evolved varieties of hypabyssal facies kimerlite.     

加氢和TSR反应对天然气同位素组成的影响

天然气形成过程中的加氢作用和 TSR 反应是有机-无机相互作用的重要方式。相邻水体和深部来源的氢,是天然气形成的重要氢源,塔里木盆地天然气的甲烷氢同位素组成明显表现出不同沉积水体对甲烷氢同位素的控制作用,大宛105～25井和阿克1井具有深部流体加氢的特征;TSR 反应中硫同位素在不同反应阶段和反应过程具有不同的分馏特征,这种特征在四川盆地高舍硫天然气中具有很好的表现,TSR 反应硫同位素分馏一般小于20‰,而单体硫、黄铁矿和硫酸盐矿物等其它反应过程的产物硫同位素分馏不明显。     

贵州红枫湖硫酸盐来源及循环过程的硫同位素地球化学研究

红枫湖是云贵高原上一个中等富营养化的季节性厌氧湖泊。对红枫湖流域湖水及其入湖河流河水一年内四个季节的水体硫酸盐硫同位素组成进行了系统研究,结果表明,红枫湖湖水硫酸盐的δ^34S值介于-8．7‰-4．9‰之间,平均-6．8‰,入湖河流的δ^34S值变化范围为-14．7‰-＋0．8‰。湖水的硫同位素组成主要受煤以及大气降水的控制,硫化物和蒸发岩的贡献较小。全年内湖水的δ^34S值季节性变化明显,表现为夏季〉秋季〉冬季、春季的特征,反映了大气降水对湖水硫酸盐贡献的季节性差异。此外,湖水垂直剖面上呈现出明显的季节性差异,冬季、春季湖水的剖面上下δ^34S值几乎没有变化,而夏季、秋季湖水表层和底层相对较高,呈规律性变化,这与湖水冬季混合、夏季分层的特点有关;夏季湖水分层期间雨水在湖泊表层的滞留,以及湖泊底层的硫酸盐细菌还原等相关生物地球化学过程是水体垂直剖面上δ^34S值规律性变化的主要原因。     

蛋白质和核糖核酸在阿哈湖沉积物中的变化特征

阿哈湖沉积物中的蛋白质和核糖核酸（RNA）随时间和沉积深度的增加逐渐被分解，其含量分别在沉积深度为17cm和19cm以后明显降低，而它们的分解产物氨基酸和核苷酸却有不同的变化规律，氨基酸在沉积深度为27－30cm的孔隙水中含量较高，这种变化规律与微生物对氨基酸和核苷酸利用的差异有关，由于地质聚合作用及矿物和有机聚合物对蛋白质的吸附作用的影响，蛋白质在沉积深度为17cm以后仍保留了一定的含量。     

贵州阿哈湖物质循环过程中的铁同位素地球化学及其指示意义

使用AGMP-1氯化物型阴离子交换树脂(100--200目)对夏季贵州阿哈湖流域水体悬浮颗粒物等样品进行了化学分离,并在多接收电感耦合等离子体质谱仪(MC-ICP-MS)上进行了铁同位素分析.分析结果表明,夏季阿哈湖湖水分层期间湖水悬浮颗粒物及各端员环境样品的铁同位素组成变化较大:湖水悬浮颗粒物的δ56Fe为负值,分布范围为-1.36‰～-0.10‰之间;各支流河水悬浮颗粒物的铁同位素组成在-0.88‰～-0.16‰之间;大气颗粒物的平均铁同位素组成为 0.06‰±0.02‰;而未经化学清洗的浮游藻类的铁同位素组成为 0.08‰.对比研究表明,湖水悬浮颗粒物的铁同位素组成不仅受各输入端员的影响,湖泊内部复杂的生物地球化学过程也对颗粒物的铁同位素组成产生了重要影响.陆源输入的颗粒有机结合态铁使得湖泊表层悬浮颗粒物的铁同位素组成偏低,而大气沉降颗粒物和湖泊表层的浮游藻类整体上对铁同位素组成的影响并不显著."ferrous wheel"铁循环对于氧化还原界面附近水层中铁同位素的重分配起到了主要的控制和影响作用.δ56Fe值与Fe/A1呈现良好的负相关关系,也显示出活性铁的循环迁移是造成氧化还原界面附近水层中悬浮颗粒物的铁同位素组成变化的重要原因,表明铁同位素与Fe/A1可能可以作为表征水体生物地球化学环境的良好指标.     

The anaerobic degradation of organic matter in Danish coastal sediments: iron reduction, manganese reduction, and sulfate reduction

We used a combination of porewater and solid phase analysis, as well as a series of sediment incubations, to quantify organic carbon oxidation by dissimilatory Fe reduction, Mn reduction, and sulfate reduction, in sediments from the Skagerrak (located off the northeast coast of Jutland, Denmark). In the deep portion of the basin, surface Mn enrichments reached 3.5 wt%, and Mn reduction was the only important anaerobic carbon oxidation process in the upper 10 cm of the sediment. In the less Mn-rich sediments from intermediate depths in the basin, Fe reduction ranged from somewhat less, to far more important than sulfate reduction. Most of the Mn reduction in these sediments may have been coupled to the oxidation of acid volatile sulfides (AVS), rather than to dissimilatory reduction. High rates of metal oxide reduction at all sites were driven by active recycling of both Fe and Mn, encouraged by bioturbation. Recycling was so rapid that the residence time of Fe and Mn oxides, with respect to reduction, ranged from 70-250 days. These results require that, on average, an atom of Fe or Mn is oxidized and reduced between 100-300 times before ultimate burial into the sediment. We observed that dissolved Mn2+ was completely removed onto fully oxidized Mn oxides until the oxidation level of the oxides was reduced to about 3.8, presumably reflecting the saturation by Mn2+ of highly reactive surface adsorption sites. Fully oxidized Mn oxides in sediments, then, may act as a cap preventing Mn2+ escape. We speculate that in shallow sediments of the Skagerrak, surface Mn oxides are present in a somewhat reduced oxidation level (< 3.8) allowing Mn2+ to escape, and perhaps providing the Mn2+ which enriches sediments of the deep basin.     

The concentration and distribution of different mercury species in the water columns and sediment of Aha Lake

In order to find out whether Aha Lake was polluted by the acid mining waste water or not, the concentration and distribution of different mercuryspecies in the water columns and sediment profile collected from Aha Lake were investigated. It was found that discernible seasonal variation of different mercury species in water body were obtained in the Aha Reservoir. With regards to the whole sampling periods, the concentrations of HgP in the Aha Reservoir water body were evidently correlated to the concentrations of total mercury, showing that total mercury was mostly associated with particle mercury. The concentrations of methylmercury in water body were also evidently correlated to the concentrations of dissolved mercury. The dissolved mercury evidently affects the distribution and transportation of methylmercury. However, there is no correlation between methylmercury and total mercury. The dissolved mercury, reactive mercury, dissolved methylmercury levels in the water body of high flow period were much higher than those in low flow period. The distribution, speciation and levels of mercury within the Aha Reservoir water body were governed by several factors, such as the output of river, the release of sediment . Discernible seasonal variation of total mercury and methylmercury in porewater was described during the sampling periods, with the concentrations in high flow period generally higher than those in low flow period. The methylmercury in pore water column was evidently correlated to that of the sediment. The results indicated that highly elevated MeHgD concentrations in the porewater were produced at the depths from 2 to 5 cm in the sediment profile, and decreased sharply with depth. A positive correlation has been found between MeHgD formation and sulfate reducing bacterial activity. These highly elevated concentrations of MeHgD at the intersurface between waters and sediments suggest a favorable methylation condition. Moreover,