贵州洪家渡水库水体不同形态汞的分布特征

通过分析贵州省乌江流域新建的洪家渡水库水体不同形态汞的浓度,探讨了水库水体各形态汞的分布特征,旨在进一步弄清新修建的水库水体汞的甲基化过程.结果表明,洪家渡水库总汞(THg)浓度变化范围在0.32～6.75 ng·L-1;溶解态汞(DHg)浓度变化范围在0.23～2.27 ng·L-1;颗粒态(PHg)汞浓度变化范围在0.03～4.51 ng·L-1;总甲基汞(TMeHg)浓度变化范围在0.04～0.18 ng·L-1;溶解态甲基汞(DMeHg)浓度变化范围在0.02～0.08 ng·L-1;颗粒态甲基汞(PMeHg)浓度变化范围在0.01～0.13 ng·L-1.洪家渡水库水体不同形态汞存在着季节性变化,水体THg、DHg和PHg的季节变化表现为夏、秋季大于春、冬季;水体TMeHg、DMeHg和PMeHg的季节变化表现为春、夏季大于秋、冬季.在空间上,水体甲基汞含量从表层到底层表现无规律性的增加趋势,从上游到下游的浓度也无明显的变化,与北美欧洲新建水库水体甲基汞浓度(0.01～6.6 ng·L-1)进行比较,发现洪家渡水库水体甲基汞浓度明显偏低,以上结果说明洪家渡水库水体没有显著的汞甲基化作用,这与乌江流域淹没土壤的贫瘠、有机质含量偏低有关.     

陕西旬阳汞矿区大气降水中汞形态分布特征

2012年7月—2013年9月对旬阳汞矿区大气降水中总汞、活性汞和溶解气态汞污染特征以及微量元素浓度进行了调查,分析了汞与微量元素浓度之间的相关性。结果表明:旬阳汞矿区大气降水中总汞、活性汞和溶解气态汞浓度的平均值分别为(48±43)、(13±9.0)和(3.8±3.6)ng·L~(-1),浓度变化范围分别为4.4~253、0.39~43和0.41~17 ng·L~(-1);大气降水中活性汞和溶解气态汞分别占总汞浓度的27%和7.9%,其他无机汞形态是其主要存在形态,占总汞浓度的65%;雨水的pH平均值为5.4,变化范围为4.2~6.7;大气降水中Hg和Sb、Se呈显著的正相关,R~2分别为0.67和0.54,说明Hg和Sb、Se具有相同的来源,其中旬阳汞矿的开采和汞锑冶炼等人为释放源为主要贡献源,其次为燃煤源。     

阿哈水库沉积物总汞及甲基汞分布特征

为弄清阿哈水库沉积物是否受到历史矿山废水输入对沉积物总汞及甲基汞垂直分布的影响,对沉积物总汞及甲基汞的含量和其垂直分布特征进行了研究.结果表明,阿哈水库沉积物总汞含量变化范围为160～252 ng·g-1,平均为210 ng·g-1,明显高于其他未受到污染的水库沉积物.沉积物中总汞含量随沉积物深度增加呈增加趋势,与其沉积环境有关.沉积物中甲基汞含量变化范围为0.2～7.2 ng·g-1,平均为1.8 ng·g-1,丰水期甲基汞含量随深度增加逐渐下降,且沉积物表层甲基汞含量显著高于枯水期,与丰水期表层有机物的增加和厌氧环境有关.     

万山汞矿区大米汞污染及人体甲基汞暴露风险

采集贵州省万山汞矿区2个流域7个地点的168个大米样品,测定其总汞及甲基汞含量,并对当地居民食用大米甲基汞暴露的健康风险进行评估。结果表明:万山汞矿区大米总汞含量变化范围为2.4~401.0 ng·g-1,平均含量为42.4 ng·g-1,51%的样品总汞含量超过我国食品汞限量标准(20 ng·g-1);甲基汞含量变化范围为1.1~45.1 ng·g-1,平均含量为11.7 ng·g-1,甲基汞占总汞的平均比例为44.8%;大米总汞与甲基汞含量呈显著正相关(r=0.44,P0.01),大米总汞含量与甲基汞占总汞的比例呈负相关(r=-0.59,P0.01)。位于河流上游离汞矿较近的地点汞污染较严重,随流域往下离汞矿较远地点汞含量相对降低。大米甲基汞暴露的风险评估显示,万山大水溪、梅子溪、白果树等污染地区存在一定的人群甲基汞暴露,而其他地区的人群也存在一定的潜在风险。     

长白山森林地区河流中汞的时空分布特征

采集并测定了枯水期和丰水期长白山北坡几条河流的水样,研究了长白山地区河流中总汞和甲基汞的时空变化规律.长白山北坡地区河流总汞的变化范围为2.0～20 ng·L-1,受北方燃煤等人为活动影响,枯水期总汞含量高于丰水期;甲基汞的变化范围为0.12～0.55 ng·L-1,不同季节的甲基汞变化不大.水体汞含量随海拔的升高而降低,汇入松花江的几条河流对松花江水体的影响较为明显,随着河流的汇入溶解态汞含量下降,颗粒态汞含量升高.与世界上其他一些森林水体对比发现,长白山水体甲基汞含量较低,但总汞含量较高.估计研究地区河流一年将向下游地区输出33 kg的总汞以及200 g甲基汞,这将进一步加剧下游水体汞的负担.     

贵州草海水生植物汞分布及其对沉积物汞的响应

以国家自然保护区草海湿地为研究对象,采集草海湖中深水区和湖边浅水区生长的主要优势植物,测定其汞和甲基汞,探讨水生植物汞和甲基汞分布特征及其对沉积物汞的响应,并评估其面临的汞污染风险。结果表明:水生植物总汞含量为5.18~40.06 ng·g-1(均值12.78 ng·g-1),与其他自然保护区报道的植物汞含量相当,其中茎叶汞含量平均值较高的有空心莲子草、小茨藻、水蓼等。水生植物甲基汞含量为0.04~2.47 ng·g-1(均值0.34 ng·g-1),其中茎叶甲基汞含量与总汞呈显著正相关性(r=0.38,n=46,P0.01)。湖边浅水区沉水植物中总汞和甲基汞平均含量均明显高于湖中深水区相同种类的植物,与沉积物中甲基汞浓度的空间分布特征一致,但与沉积物总汞空间分布特征相反,表明湖边浅水区沉积物汞的甲基化程度、生物可利用性都明显高于湖中深水区。不同采样点沉积物有机质的含量差异以及浅水区沉积物存在的干湿交替可能导致了湖中湖边植物汞和甲基汞含量的明显差异,其具体影响机制还需进一步深入研究。     

寒温带流域硅酸盐岩的风化特征——以嫩江为例

测定了嫩江水系河水主要离子组成(Ca2+、Mg2+、Na+、K+、HCO3-、SO42-、Cl-),分析了不同类型岩石风化、大气降水、人为输入对河水溶解质的相对贡献,并对整个流域以及各子流域的岩石风化速率和CO2消耗速率进行了估算.结果表明,嫩江水系河水呈弱碱性,pH平均值为7.5;阳离子以Ca2+为主,约占阳离子总量的50％;阴离子以HCO3-为主,约占阴离子总量的85％.河水中的阳离子主要来源于硅酸盐岩风化(约38％)和碳酸盐岩风化(约32％),其余来源于蒸发岩溶解(约25％)和人类活动(约5％)以及大气降水输入(＜1％).嫩江流域硅酸盐岩风化速率约为1.37 t· km-2·a-1(TDS硅酸盐岩),硅酸盐岩风化对大气CO2的消耗速率约为40.1×103 mol·km-2·a-1.     

贵州百花湖鱼体汞污染现状

以西南汞污染严重的贵州百花湖为对象,选取湖中优势鱼、贝类,通过测定其总汞和甲基汞含量,并结合水体、沉积物汞含量和相关水质参数,探讨了百花湖鱼类汞污染的现状及其影响因素.百花湖鱼体总汞平均含量为28.0ng·g-1,变化范围为4.2～143ng·g-1;甲基汞的平均含量为10.9ng·g-1,变化范围为3.0～39.3ng·g-1.虽然百花湖遭受上游贵州有机化工厂含汞废水的严重污染,但鱼体汞含量并没有超过国家食品卫生标准.其主要原因可能是:百花湖的鱼主要是人工养殖的草食性或杂食性鱼类,鱼龄较小,且其摄取的食物汞含量低、食物链简单,不利于汞的富集;其次,其较快的生长速度对鱼体汞具有生物稀释的作用.     

九龙江丰水期水化学组成特征及其控制因素

为了解九龙江流域水环境状况,于2017年7月对福建九龙江河水样品进行了系统采集与分析。结果显示,九龙江丰水期河水pH在6.7~7.9,平均7.2,呈弱碱性;TDS平均含量为90.9 mg·L-1,低于世界河流平均值。电导率(EC)和溶解氧(DO)的平均值分别为116.5μS·cm-1和7.5 mg·L-1。水化学类型为HCO3-SO4-Ca型,Ca2+是主要的阳离子,占阳离子总量的47.9%,K+和Na+二者之和占总阳离子的29.6%。HCO3-和SO42-是主要的阴离子,二者之和占阴离子总当量的68.6%。采用正演法估算各端元贡献,显示碳酸盐岩和硅酸盐岩风化是九龙江水化学组成的主要控制因素,对河水总阳离子的贡献分别为50.6%和30.7%。大气降水对九龙江流域影响较大,约贡献了阳离子总量的12.9%。人为活动对河水的化学组成影响也不容忽视,特别是对SO42-和NO3-的含量影响较大。九龙江工农业布局使得北溪河水主要受工业生产影响,而西溪和南溪主要受农业活动影响。因此,在治理九龙江水环境时,除了严格控制城镇污水排放外,北溪还需加强工业废水管理,而西溪和南溪要严格控制农田化肥的使用。     

网箱养鱼对水库水体甲基汞的影响

分别在2010年9月(暖季)和2011年3月(冷季),选取乌江渡水库网箱养鱼区和距离网箱100～200m的对照区(库心),对水体不同形态汞及其他相关参数进行了研究,以揭示网箱养鱼对水库汞地球化学行为的影响。结果表明,暖季养鱼区水体总汞含量为(2.04±0.53)ng·L-1,甲基汞含量为(0.146±0.231)ng·L-1,对照区水体总汞含量为(3.33±2.39)ng·L-1,甲基汞含量为(0.380±0.577)ng·L-1;冷季养鱼区水体总汞含量为(3.04±1.53)ng·L-1,甲基汞含量为(0.047±0.028)ng·L-1,对照区水体总汞含量为(3.24±1.23)ng·L-1,甲基汞含量为(0.046±0.013)ng·L-1;养鱼区与对照区总汞含量(n=35,P=0.875)、甲基汞含量(n=35,P=0.091)均无显著差异。结合对养鱼区与对照区水体中其他各参数(总氮、总磷、溶解性有机碳、叶绿素、温度、溶解氧等)综合分析表明,由于水库蓄水与泄水发电对水库水体的扰动及水库自身水体的交换作用导致水体呈混匀状态,网箱养鱼造成的水体甲基化程度差异不显著;而水库水体季节性分层造成的水体底部厌氧和温度的变化是影响水体甲基汞含量及分布的主要因素之一。     

长白山北坡森林土壤汞的含量和形态分布

分别于2009年4月和9月对长白山北坡的土壤样品进行了采集,研究北方森林地区不同海拔土壤样品中的总汞和甲基汞的分布情况.长白山土壤THg和MeHg含量分别为0.08～0.73 mg·kg-1和0.05～0.56 μg·kg-1,库存量分别为97 kg·km-2和128 g·km-2,高于吉林省背景值,MeHg的最高含量...     

Genetic engineering of bacteria and their potential for Hg2+ bioremediation

Ion exchange or biosorptive processes for metalremoval generally lack specificity in metal bindingand are sensitive to ambient conditions, e.g. pH,ionic strength and the presence of metal chelators. Inthis study, cells of a genetically engineered Escherichia coli strain, JM109, which expressesmetallothionein and a Hg²⁺ transport system afterinduction were evaluated for their selectivity forHg²⁺ accumulation in the presence of sodium,magnesium, or cadmium ions and their sensitivity to pHor the presence of metal chelators during Hg²⁺bioaccumulation. The genetically engineered E.coli cells in suspension accumulated Hg²⁺effectively at low concentrations (0-20 µM) overa broad range of pH (3 to 11). The presence of 400 mMsodium chloride, 200 mM magnesium chloride, or100 µM cadmium ions did not have a significanteffect on the bioaccumulation of 5 µm Hg²⁺,indicating that this process is not sensitive to highionic strength and is highly selective against sodium,magnesium, or cadmium ions. Metal chelators usuallyinterfere with ion exchange or biosorptive processes.However, two common metal chelators, EDTA and citrate,had no significant effect on Hg²⁺ bioaccumulationby the genetically engineered strain. These resultssuggest that this E. coli strain could be usedfor selective removal of Hg²⁺ from waste water orfrom contaminated solutions which are resistant tocommon treatments. A second potential applicationwould be to remove Hg²⁺ from Hg²⁺-contaminated soil, sediment, or particulates bywashing them with a Hg²⁺ chelator andregenerating the chelator by passing the solutionthrough a reactor containing the strain.     

Long-term performance of bioreactors cleaning mercury-contaminated wastewater and their response to temperature and mercury stress and mechanical perturbation

The long-term performance of bioreactors retaining mercury from contaminated industrial wastewater was analyzed at the laboratory scale, and its response to mechanical perturbations (gas bubbles and shaking) as well as to physical (increased temperature and hydraulic load) and chemical stresses (increased mercury concentration) likely to occur during on site operation was studied. Two packed-bed bioreactors with 80-cm(3) lava chips as biofilm carrier were inoculated with nine Hg(II)-resistant natural isolates of alpha- and gamma-proteobacteria. Chloralkali wastewater containing ionic mercury (3.0 to 9.7 mg/L Hg(2+)), amended with sucrose and yeast extract, flowed through the bioreactors at 160 mL/h. During the 16-month investigation the bioreactors showed no sign of depleted performance in terms of mercury-retaining capacity. After 16 months, both bioreactors still retained 96% of the mercury load. The performance of the bioreactors was sensitive to mechanical perturbations (e.g., sheer forces of gas bubbles). Shifts to higher Hg(2+) inflow concentrations initially decreased the mercury retention efficacy slightly. However, the bioreactors could adapt to Hg(2+) concentrations of up to 7.6 mg/L within several days. Old biofilms were less affected than the younger ones. The performance of the bioreactors was not affected by an increase in temperature up to 41 degrees C and an increased volumetric load (up to 240 mL/h). The bioreactors regained activity spontaneously after the stress had stopped. Recovery could be accelerated by increased nutrient concentration, although this may lead to blocking of the packed bed.     

Diel variability of mercury phase and species distributions in the Florida Everglades

Preliminary studies of mercury (Hg) cycling in the Everglades revealed that dissolved gaseous mercury (DGM), total mercury (Hg_T), and reactive mercury (Hg_R) show reproducible, diel trends. Peak water-column DGM concentrations were observed on or about noon, with a 3 to 7 fold increase over night-time concentrations. Production of DGM appears to cease during dark periods, with nearly constant water column concentrations that were at or near saturation with respect to the overlying air. A simple mass balance shows that the flux of Hg to the atmosphere from diel DGM production and evasion represents about 10% of the annual input from atmospheric deposition. Production of DGM is likely the result of an indirect photolysis reaction that involves the production of reductive species and/or reduction by electron transfer. Diel variability in Hg_T and Hg_R appears to be controlled by two factors: inputs from rainfall and photolytic sorption/desorption processes. A possible mechanism involves photolysis of chromophores on the surface of a solid substrate (e.g., the periphyton mat) giving rise to destabilization of sorbed mercury and net desorption during daylight. At night, the sorption reactions predominate and the water-column Hg_T decreases. Methylmercury (MeHg) also showed diel trends in concentration but were not clearly linked to the solar cycle or rainfall at the study site.     

System controls on the aqueous distribution of mercury in the northern Florida Everglades

The forms and partitioning of aqueous mercury species in the canals and marshes of the Northern Florida Everglades exhibit strong spatial and temporal variability. In canals feeding Water Conservation Area (WCA) 2A, unfiltered total Hg (HgT_U) is less than 3 ng L^-1 and relatively constant. In contrast, methyl mercury (MeHg) exhibited a strong seasonal pattern, with highest levels entering WCA-2A marshes during July. Stagnation and reduced flows also lead to particle enrichment of MeHg. In the marshes of WCA-2A, 2B and 3A, HgT_U is usually <5 ng L^-1 with no consistent north–south patterns. However, for individual dates, aqueous unfiltered MeHg (MeHg_U) levels increase from north to south with generally lowest levels in the eutrophied regions of northern WCA-2A. A strong relationship between filtered Hg species and dissolved organic carbon (DOC), evident for rivers draining wetlands in Wisconsin, was not apparent in the Everglades, suggesting either differences in the binding sites of DOC between the two regions, or non-organic Hg complexation in the Everglades.     

酸沉降地区大气汞对土壤-植物系统汞累积影响的调查研究

按酸沉降危害程度的差异及不同功能区,进行了大气、植物、土壤汞的同步调查采样分析。结果表明,大气汞对土壤－植物系统汞累积的影响非常明显,土壤、植物含汞量均随大气汞浓度的升高而升高,土壤－植物系统汞累积与大气汞浓度有显著的相关（相关系数分别为ｒ植＝０．８８２＊＊,ｎ＝５３;ｒ土＝０．７４１＊＊,ｎ＝５２）。调查还发现,当大气汞浓度大于３０ｎｇ／ｍ３时,土壤－植物系统汞累积较为明显,因此把３０ｎｇ（Ｈｇ）／ｍ３作为本地区大气汞对土壤－植物系统造成二次污染的临界浓度     

Sulfate-reducing Bacteria and Mercury Methylation in the Water Column of the Lake 658 of the Experimental Lake Area

Sulfate-reducing bacteria (SRB) appear to be the main mediators of mercury methylation in sediments, which are deemed to be major sites of methylmercury (MMHg) production. However, recent studies have also found significant MMHg formation in the water column of lakes across North America. To investigate the potential involvement of SRB in mercury methylation in the water column of a stratified oligotrophic lake, two of the main families of SRB (Desulfobacteraceae and Desulfovibrionaceae) were quantified by Real-Time Polymerase Chain Reaction of the 16S rRNA gene. MMHg production was measured applying a stable isotope technique using ¹⁹⁸HgCl. Methylation assays were conducted at different water depths and under stimulation with lactate, acetate or propionate and inhibition with molybdate. Desulfobacteraceae and Desulfovibrionaceae16S rRNA gene copies in control samples accounted for 0.05% to 33% and <0.01% to 1.12% of the total bacterial 16S rRNA, respectively. MMHg formation was as high as 0.3 ng L^?1 day^?1 and largest in lactate amended samples. Strain isolation was only achieved in lactate amended media with all isolated strains being SRB belonging to the Desulfovibrio genus according to their 16S rRNA gene sequence. Isolated strains methylated between 0.06 and 0.2% of ¹⁹⁸HgCl per day. Acetate and propionate did not stimulate mercury methylation as much as lactate. Two strains were identified as Desulfovibrio sp. 12ML1 (FJ865472) and Desulfovibrio sp. 12ML3 (FJ865473), based on partial sequences of their 16S rRNA and DSR gene. Methylation assays and bacteria characterization suggest that Desulfovibrionaceae is an important mercury methylators in Lake 658. Supplemental materials are available for this article. Go to the publisher's online edition of Geomicrobiology Journal to view the free supplemental file.     

五里河沉积物汞的时空变化规律

研究了历史上受纳氯碱污染的辽宁省葫芦岛市五里河沉积物中总汞、甲基汞25年中的时空变化规律.结果表明,经过25年的变化,在人工治理和自然净化作用下,五里河不同地点沉积物总汞和甲基汞含量总体上呈现明显下降的趋势,甲基汞下降尤为显著;但沉积物中汞含量依然处于较高水平,总汞含量为0.491～26.395 mg·kg-1,平均13.766 mg·kg-1,超过辽宁省土壤汞背景值(0.037 mg·kg-1)371倍,甲基汞含量为0.253～12.079 μg·kg-1,污染严重的断面是污染源附近的化工桥以及下游河口附近的茨山北桥.     

The Influence of Long-term Mercury Exposure on Selenium Availability in Tissues: An Evaluation of Data

The precise mechanisms of mercury accumulation and retention are still unclear. Generally, the association of mercury with selenium is used to explain these phenomena. It seems that the presence of coaccumulated endogenous Se can protect cells from the harmful effects of Hg. However, as speculated by some authors, this binding of Se to Hg can also result in a relative deficiency of biologically available Se needed for selenoenzyme syntheses. Deriving from the assumption that Hg deposited in tissues is bound to Se in a 1:1 ratio, the quantity of non-Hg bound Se could be calculated by the difference between the molar contents of the two elements (Se_mol–Hg_mol). In this study we applied such an approach to the data from our previous investigation, where Hg and Se concentrations were determined in autopsy samples of mercury exposed retired Idrija mercury mine workers, Idrija residents living in a Hg contaminated environment and a control group with no known Hg exposure from the environment. Based on these data we tried to estimate the influence of Hg exposure on the physiologically available selenium content in selected tissues, particularly endocrine glands and brain tissues. Comparing the calculated values of (Se_mol– Hg_mol) it was found that for Idrija residents the values were similar to those of the control group and as expected, diminished values were found in some mercury-loaded organs of retired Idrija miners. It could be speculated that in Idrija residents Hg sequestration of selenium is sufficiently compensated by increased Se levels, but that particularly in active miners and in some organs of retired miners, the activity and/or synthesis of selenoenzymes could be disturbed. Part of the study was presented at the 7th International Conference on Mercury as a Global Pollutant, June 27–July 2, 2004 Ljubljana, Slovenia (Falnoga et al. 2000)