Distribution and speciation of mercury in surface water in Wanshan Hg-mined areas, Guizhou Province, China

Mercury as a toxic element poses environmental concerns, especially in historically Hg-mined districts. The Wanshan Hg mine located in the eastern part of Guizhou Province, southwestern China, ranks the largest Hg-producing district in China. Mining at Wanshan was initiated in 221 B.C., but ceased in 2001. Approximately 22000 tons of Hg, 6000 tons of cinnabar and large quantities of mine-wastes had been produced at Wanshan. Significant quantities of calcines, which were piled irregularly near the old mine processing sites and retorts, continue to impact the local environments in the Wanshan area. In this study, a regional contamination of mercury in surface waters collected from the Meizixi, Dashuixi, Huandao and Gaolouping rivers, whose upstreams or branches originate from the hilly karstic area and receive drainage arising from the calcines, was investigated by determining all Hg species in a base-flow and a flood-flow season. Reactive, dissolved, particulate, and total Hg concentrations in surface water varied from 0.60 to 400 ng/L, 11 to 430 ng/L, 1.4 to 9210 ng/L, and 15 to 9260 ng/L, respectively. Total methylmercury in water samples ranges from 0.31 to 25 ng/L. The concentrations of total Hg and particulate Hg in water samples collected during the flood season are higher than those in the base-flow season, whereas, the concentrations of dissolved and reactive Hg are lower with the peak values observed in water samples collected in the base-flow season. A strong positive correlation between total Hg and particulate Hg is noticed in the water samples collected from Hg-mined areas with the proportion higher than 80%.     

Distribution and speciation of mercury in the Hongfeng Reservoir,Guizhou Province,China

The water, pore water, sediment, and fish samples were collected from the Hongfeng Reservoir in November 2003 and February 2004 in accordance with trace metal protocols. The average concentrations of total mercury （THg）, dissolved mercury （DHg）, reactive mercury, dissolved gaseous mercury, total methylmercury, and dissolved methylmercury in the water columns were 8.00, 5.70, 0.63, 0.05, 0.16, and 0.07 ng/L, respectively. THg and DHg in the water columns, THg in pore water and THg in lake sediments of the Hongfeng Reservoir showed the level of mercury in the Hongfeng Reservoir was higher than in other natural waters in the world due to the loading of a lot of waste water with relatively high concentrations of mercury, whereas methylmercury concentrations in fish （wet weight） varied from 1.73-51.00 ng/g, much lower than in most remote lakes and reservoirs reported in northern Europe and North America. Methylmercury distributions in pore water and sediments showed methylation occurred mainly in the upper several centimeters of sediment cores in the Hongfeng Reservoir. The concentrations of dissolved organic carbon, total suspended particles, total Hg, and methylmercury were higher at Houwu than those at Daba in November 2003. It is suggested that other pollutants such as N and P from fishing farm and other waste water at Houwu, which resulted in deterioration of water quality, affected the concentrations and distributions of mercury species in the reservoir.     

Methylmercury and total mercury distribution in the sediments of Baihua Reservoir, Guizhou Province, China

Mercury is an important pollutant in lakes. Methylmercury （MeHg）, the most toxic mercury species, which can be formed from inorganic mercury in lakes, can be bioaccumulated into high concentration in food chain and result in a potential threat to human beings. Sediments play an important role for the Hg biogeochemistry in the aquatic systems： Mercury methylation has been shown to be fastest in the surfacial sediments, where the microbial activity is highest. The formation of MeHg in lakes suggests that sediments and/or near-shore wetlands can be the sources of MeHg in aquatic environments. The Baihua Reservoir, located in the suburb of Guiyang, was impounded in 1966. From the 1970s to the 1990s, Guizhou Organic Chemical Plant which used inorganic mercury as catalyst to produce acetic acid, was responsible for the discharge of waste water with high mercury content.     

Research on the carbon isotopic composition of organic matter from Lake Chenghai and Caohai Lake sediments

The carbon isotopic composition of organic matter from lake sediments has been extensively used to infer variations in productivity. In this paper, based on the study of the contents and δ13C values of organic matter in different types of lakes, it has been found that δ13C values of organic matter have different responses to lake productivity in different lakes. As to the lakes dominated by aqutic macrophytes such as Lake Caohai, organic matter becomes enriched in 13C with increasing productivity. As to the lakes dominated by aquatic algae such as Lake Chenghai, δ13C values of organic matter decrease with increasing productivity, and the degradation of aquatic algae is the main factor leading to the decrease of δ13C values of organic matter with increasing productivity. Therefore, we should be cautious to use the carbon isotopic composition of organic matter to deduce lake productivity.     

贵州草海近21 ka以来有机地球化学记录反映的古环境变化*

草海位于黔滇交界,主要受印度夏季风的影响,其湖沼沉积物记录了中—晚第四纪的环境变化历史,是研究第四纪环境和季风演变的良好载体。本研究选取的南屯NT03钻孔,岩心长405 cm,在放射性碳同位素(AMS¹⁴C)测年基础上建立了年代序列,并进行了沉积物的色差值(L^*)、烧失量(LOI550)、总有机碳(TOC)、碳氮比(C/N)和有机稳定碳同位素(δ13Corg)等古环境替代指标的测试。实验结果显示,L^*、LOI550和TOC等3个有机碳含量指标同步变化,共同指示该钻孔序列经历了3个沉积环境演变阶段,即末次盛冰期晚期(21—15 cal ka BP)河流—冲积相沉积阶段、冰消期至早中全新世(15—4 cal ka BP)高湖面湖泊—沼泽相沉积阶段和晚全新世(4 cal ka BP以来)洪冲积相沉积阶段。近2万年以来草海湖沼面积经历的收缩→扩张→收缩演变过程与石笋氧同位素变化基本吻合,表明季风降雨是引起草海湖泊水体和周边生态系统变化的主要因素。δ13Corg指标变化范围为-29.28‰~-24.19‰,表明草海盆地周围植被组成在末次盛冰期以来C4草本虽然略有增加,但均以C3植物为主。同时,TOC和δ13Corg指标证明了B/A冰消期暖事件对盆地边缘区的湿地泥炭富集起到关键作用,而多指标揭示了近4 ka以来水域变浅并发展成为冲积环境的过程,也可能与石笋记录的夏季风减弱所带来的降水量减少有关。     

贵州草海赵家院子晚更新世泥炭层地球化学特征及其环境意义

根据威宁草海赵家院子沉积柱主量元素和微量元素特征以及14C测年分析,探讨了草海地区泥炭沉积速率,晚更新世—全新世古气候演变和沉积物物源环境。元素地球化学测试结果表明,Li、Sc、V、Cr、Ni、Ga、Rb、Sr、Sn、Cs、Ba、Zr、Th、U等14种微量元素在沉积柱上含量变化整体呈现一致性。14C测年显示,赵家院子剖面沉积柱下部泥炭层的年龄大约为33.74±1.79—23.29±0.10kaBP之间,各层的沉积速率自下而上分别是:下部泥炭层148.4mm/ka,上部黑色古土壤层24.3mm/ka,顶部堆积层22.4mm/ka,沉积柱沉积速率由下而上逐渐降低。元素对比值以及多元素之和比值Sr/Ba、Rb/Sr、(CaO+K2O+Na2O)/Al2O3、(Fe2O3+Al2O3)/(MgO+CaO)和CaO/MgO等气候指标显示,从42.37±1.27kaBP到15.6±0.1kaBP时间段内,研究区古气候经历了由温暖较湿润→温暖湿润→温凉干燥→温暖较湿润→温凉湿润的演化。沉积物物源经历了较强烈的化学风化,下部泥炭层风化程度小于上部沉积物的风化程度。     

太湖及其主要入湖河流沉积磷形态分布研究

选择了我国第三大浅水湖泊--太湖及其主要入湖河流进行沉积磷形态的连续提取研究.太湖湖区沉积磷中不稳态磷(LP)及铝结合态磷(Al-P)含量很低,其余形态磷为铁结合态磷(Fe-P)＜钙结合态磷(Ca-P)＜有机磷(Org-P).河流沉积物中有机磷的相对含量高于湖泊沉积物,绝对含量平均值约为湖泊沉积物的3.9倍,铁结合态磷的绝对含量约为湖泊沉积物的3/4,湖区沉积物Fe-P含量与水体中PO3-4-、Chla呈显著正相关关系,同时与间隙水的氧化性呈显著负相关关系.太湖各湖区沉积物的磷形态表现为空间差异较大,活性组分的差异性要大于活性较差的组分.总的来说北部湖区沉积物中Fe-P和Org-P含量高于其他湖区,这与太湖北部湖区水体高营养级和藻类爆发关系密切.湖区沉积磷的垂直分布规律较复杂,既有随深度增加的,也有随深度降低的,河流沉积物同样如此.这与太湖及河流生态条件、污染物排放以及沉积动力学条件不同有关.     

Spatial and temporal distributions of mercury species and controlling factors in Hongfeng Reservoir, Guizhou, China

The Hongfeng Reservoir was built in 1960 and is an alkaline, hyper-eutrophic and seasonal anoxic reservoir due to the contamination from domestic and industrial wastewaters. The water samples at deferent depths from two sampling sites were collected from November 2003 to September 2004 using metal clean protocols. Total Hg （THg）, reactive Hg （RHg）, dissolved total Hg （DHg）, dissolved gaseous mercury （DGM） were measured by gold trap pre-concentration and CVAFS detection. Methyl mercury was measured by distillation followed by aqueous phase ethylation, precollection on a Tenax, isothermal gas chromatography and cold vapor atomic fluorescence detection. There was no discernible seasonal trend （about 8 ng/L） in THg concentration based on the average information developed during the four cruises except for high concentrations at bottom and water-sediment interface in May and September 2004. On the other hand, particulate mercury （PHg） and methyl mercury have discernible seasonal variability. Proportion of PHg increased from 29% in February 2004 to 50% in May 2004. In November 2003, February and May 2004 methyl mercury concentrations were relative low and increased with depth （from 0.13 to 0.40 ng/L）. In September 2004, methyl mercury concentrations increased from 0.14 ng/L in the epilimnion to 0.99 ng/L in the hypolimnion. DGM concentrations varied from 0.024 to 0.11 ng/L and decreased with depth.     

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,     

贵州威宁窑上组沉积物物源特征及沉积控制因素分析

根据威宁草海第四纪窑上组沉积物主量元素和REE特征,探讨沉积物物源特征、气候演变情况、沉积物堆积控制因素。结果表明:Al、Mg、Ca、K、Na和Ti的含量变化在剖面上一致,它们的相关系数很高(0.522~0.985)。Fe含量和Mn含量呈正相关形式,与Al、Mg、Ca、K、Na和Ti呈负相关。Fe2O3含量在土黄色粘土的铁质层很高(42.86%~50.57%)。样品中REE球粒陨石标准化配分模式与贵州土壤、贵州碳酸盐岩风化壳配分模式很相似,与峨眉山玄武岩配分模式不一致,但其含量略低于贵州碳酸盐岩风化壳的含量;沉积物主要来源于碳酸盐岩,且碳酸盐岩强烈风化成土作用使REE超常富集,在剖面上呈现高ΣREE(平均219.38μg/g)。通过Mg/Ca、MgO/Al2O3、(CaO+K2O+Na2O)/Al2O3、(Fe2O3+Al2O3)/(MgO+CaO)、(K+Na+Ca+Mg)/(Fe+Mn)、(Al+Fe+Mn)/(K+Ca+Mg)和(MgO+Na2O+CaO)/Al2O3等气候指标研究,表明在草海窑上期为湖泊沉积时期,气候经历了由温暖湿润向冷干的转变。同时,认为物源性质、构造运动、气候等共同控制该区沉积物形成。     

湖南洞庭湖水系As和Cd等重金属元素分布特征及输送通量

土壤地球化学调查显示,长江沿岸,尤其湖南洞庭湖流域存在以镉为主的重金属高值带。为进一步确定As和Cd等重金属元素在河流中的存在形式、迁移方式和通量等地球化学特征,本研究在洞庭湖水系主要干支流的关键位置布置采样点,分夏季丰水期和冬季枯水期两次,采集了原水、0.45μm过滤水和0.20μm过滤水等水样品,以及悬浮物固体样品,分析了水和悬浮物样品中As和Cd、Pb等重金属元素含量。结果发现,As元素在湘江、资水、湘江上游支流西河和耒水中含量最高,耒水、西河及湘江的Pb、Zn含量相对偏高,Cd在湘江、耒水及汨罗江的含量也明显高于其他河流;研究区河水中As、Ni、Cd和Zn等元素在水中离子态比例较大,其溶解态含量受河水pH和温度的控制,湘江、西河、耒水和汨罗江中悬浮物As、Zn、Cu、Cd、Pb和Cu等元素含量远高于其他水系悬浮物,这与这些流域内存在多金属矿区密切相关;不同元素在河水中迁移途径有很大差别,As以溶解态和胶体态为主要迁移形式,Pb、Zn、Cu、Cd和Ni等重金属元素以悬浮物形式迁移的比例最大;主要入湖河流中,湘江输入洞庭湖的As、Zn、Cu和Cd总量最大,年通量分别为961.43 t、478.90 t、101.67 t、59.58 t。     

南海湖沉积物中Hg的形态分布特征

以包头市南海湖为研究对象,采用连续化学提取法,系统开展了沉积物中Hg的形态分布研究。结果表明,表层沉积物中Hg含量的水平分布总体呈现湖心区低,西南和东北部湖区高的趋势。腐殖酸结合态为表层沉积物中Hg的主导形态,次为交换态和水溶态。表层沉积物中生物有效态Hg的含量甚高,占总汞的76%~94%,对整个生态系统具有潜在危害性。沉积柱芯中总Hg表现为表层富集并随深度增加而降低的变化趋势。B、F站位柱状沉积物中腐殖酸结合态Hg随深度有规律的递减,H站位20 cm以上Hg的主导形态为腐殖酸结合态,残渣态次之;20～30 cm的主导形态则为残渣态及可交换态。     

Human Influence on Heavy Metal Distribution in the Upper Lake Nansi Sediments, Shandong Province, China

Core and surface sediment samples were collected from three sub-lakes ( Lake Nanyang, Lake Dushan and Lake Zhaoyang) in the Lake Nansi Basin, Shandong Province. In order to reveal the characteristics of spatial and historical distribution of heavy metals in different sublakes of the Upper Lake Nansi, heavy metal (As, Cr, Cu, Hg, K, Mn, Ni, Pb, Zn, Al, Fe, Ti and V) concentrations of sediment samples were investigated. Based on the activity of^137Cs in the sediments, the modem accumulation rate of Lake Nansi sediments is 3.5 mm/a. Our results show that the whole Upper Lake Nansi has been already polluted by heavy metals, among which Lake Nanyang has been polluted seriously by mercury, as well as by lead and arsenic, while Lake Dushan has been most seriously polluted by lead and arsenic. Historical variation of heavy metal (Cr, Cu, K, Ni, Zn, A1, Fe, Ti and V) concentrations shows an abrupt shift in 1962, resuiting in a division of two periods: from 1957 to 1962 when metal enrichment increased with time, and from 1962 to 2000 when it decreased with time, while that of some anthropogenic elements such as Hg, Pb and Mn tend to increase toward the surface. However, the variation trend of As in the sediments is different from that of Hg, Pb and Mn, with its maximum value appearing in 1982. Since 1982 the concentrations of As have decreased due to the forbidden use of arsenite pesticides. This variation trend revealed changes in manner of human activity (coal combustion, waste discharges from both industries and urban sewage ) within the catchment during different periods.     

Sediment particle size distribution and its environmental significance in Lake Erhai, Yunnan Province

A closed or semi-closed plateau lake, whose sediment records can provide us with plenty of fine and high resolution information, is a sensitive indicator of climatic and environmental changes. During the reconstruction of various short-time-scale climatic and environmental changes, the geochemical records in plateau-lake sediments are superior to other natural files. Based on fine dissection of the vertical profile of sediment particle sizes, this paper reveals the quasi-periodical changes of sediment particle sizes, which indicates the quasi-periodical fluctuations of the regional climate. A synthetic analysis of multiple indexes shows that sediment particle size is a more sensitive and more effective index of climatic and environmental changes than other geochemical indexes. High content of >20μm sediment particles and low content of 2–10μm sediment particles indicate a warm-dry climate and conversely a cold-humid climate, and their ratio can be used as an effective index of climatic changes. The basic climate succession in the region of Lake Erhai is characterized as being alternatively warm-dry and cold-humid and it has been developing into a warm-dry climate as a whole. There exist at least 2 time-scale quasi-periodical fluctuations of the regional climate in Lake Erhai. At present, the region of Lake Erhai is at the end of the warm-dry period and at the beginning of a cold-humid period, so the temperature will go down and the water level will rise. This project was supported by the National Natural Science Foundation of China (Nos. 49894170, 49773207).     

云南星云湖表层沉积物粒度空间分布特征及其影响因素

本文以滇中地区星云湖为研究对象,对湖区84个表层沉积物样品进行了粒度测定,并进行了参数计算和空间分布特征分析,进而探讨了星云湖表层沉积物粒度的环境及人类活动指示意义。结果表明：星云湖表层沉积物平均粒径在8.82~57.71 μm之间,粉砂为该研究区的优势粒级,平均含量达到62.48%,粘土和砂含量的平均值分别为30.68%和7.04%。研究区北部受入湖河流的影响,砂含量较高;南部由于受到盛行风、湖流和湿地的影响,呈现为舌状细粒沉积为主;在其东部螺蛳铺河入湖区,由于受到湖流的顶托作用和人类农耕和河道改造的影响,粉砂和粘土含量较高。星云湖表层沉积物除海门村附近外普遍较细、整体分选极差,而在北部湖区表现为正偏态。河流入湖口沉积物粒度参数表现出不同特征,其中北部入湖口呈单主峰和多峰态的组合特征,东部入湖口呈双峰态,西南各入湖口呈单、双峰组合特征。星云湖现代沉积物与沉积环境和物源的变化紧密相关,是研究湖泊沉积和环境变化的理想场所。

     

Mercury emission from the indigenous mercury smelting in Wuchuan mercury mining areas, Guizhou Province, China

Mercury smelting is one of the important anthropogenic atmospheric mercury emission sources. Small-scale mercury smelting activities with indigenous method which is considered illegal and forbidden by local government always extensively existed in the Wuchuan area, northeastern Guizhou Province, China. Because of the simple processes without any environmental protection, a large amount of mercury vapor released to the ambient air during the processing of cinnabar roasting. By determining mercury concentrations in mercury ore and smelting slag samples, a mass balance method was used to calculate mercury emission factors and annual mercury emission from indigenous mercury smelting in Wuchuan mercury mining areas, Guizhou Province, China. The mercury emission factors ranged from 6.9% to 32.1% with the recovery from 78.4% to 93.6% and the annual mercury emission was up to 3.7-9.6 metric tons. The results highlighted that the indigenous mercury smelting was one of the most important anthropogenic atmospheric mercury emission sources in this region.     

Seasonal distribution of total mercury and methylmercury in sediments of the Wujiangdu Reservoir, Guizhou, China

The concentrations of total mercury and methylmercury in sediments were determined at the dam of the Wujiangdu Reservoir in different seasons. Total mercury (HgT) levels in the whole sediment profile were 254.2±47.0 ng/g in winter, 254.2±31.6 ng/g in spring, and 256.7±60.8 ng/g in summer, without significant variations in different seasons or at different depths. In contrast, the methylmercury (MeHg) compounds were most abundant at the sediment-water interface and decreased progressively with depth. MeHg contents of the sediments during different seasons are highly dependent on microbial activity, and seem to be higher when Hg (II)-methylating microorganisms are active. Thus, MeHg levels tend to rise in the loci where nutrient supplies and biological productivity are favorable. The percentage of HgT that is present as MeHg in the sediments increased gradually from December 2003 to April 2004 and to July 2004.     

内蒙古岱海表层沉积物中孢粉的分布及来源

岱海位于半干旱区东部边缘及东亚夏季风的尾闾区，生态环境体系脆弱，气候和环境变化敏感，是研究环境变化的理想地区。65个湖泊表层及入湖河流冲积物样品的孢粉分析揭示了岱海表层孢粉沉积特征及孢粉来源。岱海表层孢粉主要来源于区域性植被的孢粉，其总体特征反映了区域植被的组成，但不同部位孢粉组合的差异反映了湖滨当地植被的变化。受沉积环境的影响，岱海湖区孢粉浓度总体上要低于入湖河流孢粉浓度，湖区中部孢粉浓度最高。岱海孢粉以河流携带的为主，同时受风力传播的影响。蒿、藜科、桦、虎榛子等花粉和蕨类孢子以河流搬运的为主，松、禾本科及莎草科花粉可能还受风力传播的影响。一些仅在个别样品中出现且百分比很低的花粉类型如豆科、十字花科等还有可能是昆虫、鸟类或人类活动携带而来。     

南盘江上游草海断陷盆地岩溶水系统研究

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