万山汞矿区稻田土壤甲基汞的分布特征及其影响因素分析

运用等温气相色谱冷原子荧光技术(GC-CVAFS)对贵州万山汞矿区主要河流范围内稻田土壤甲基汞(MeHg)等含量进行了测定,并从区域层面对土壤甲基汞(MeHg)的分布特征及影响因素进行了研究。结果表明:万山汞矿区稻田土壤MeHg和总汞(THg)含量范围分别为0.72~6.70ng/g和0.49~188.00μg/g,甲基化率范围为0.002%~0.470%;在水平空间分布上,6个检测区域的土壤MeHg含量均随着远离汞矿核心区而降低,但是不同区域之间的降低变化程度不尽相同。通过对稻田土壤SiO2、Al2O3、Fe2O3、TS、TP、TN、有机质、pH等土壤性质与土壤MeHg以及甲基化率进行相关性分析发现,MeHg与THg、TS、TP、TN、有机质存在显著的正相关关系,与SiO2表现出显著性负相关,表明土壤甲基汞不但和总汞含量有关,还受到土壤其它理化因子,尤其是一些营养因子所控制。     

大连湾表层沉积物中总汞和甲基汞的分布及影响因素

为研究大连湾表层沉积物中THg（总汞）和MeHg（甲基汞）的分布及影响因素,于2016年7月对大连湾12个采样点表层沉积物进行了调查,分析了沉积物中w（THg）和w（MeHg）及其与环境因子的关系.结果表明:①大连湾表层沉积物中w（THg）和w（MeHg）的平均值分别为（79.5±47.1）和（0.53±0.26）ng/g,MeHg%（甲基化比率）范围为0.39%~1.46%,平均值为0.74%.②沉积物中w（THg）和w（MeHg）均表现出由湾内向湾外降低的趋势,而MeHg%的空间分布特征与w（THg）和w（MeHg）相反,并且水产养殖活动的外源输入也可对MeHg%产生影响.③w（MeHg）与各环境因子均呈显著相关关系,表明沉积物中w（MeHg）主要受w（THg）和氧化还原条件的影响;MeHg%与Hg/C（THg与TOC摩尔比,下同）呈显著负相关,可能主要与沉积物中生物可利用Hg的比例影响有关,而MeHg%虽然与w（TOC）、w（TS）的相关性均不显著,但也体现出有机质和硫对Hg的生物可利用性的影响.研究显示,沉积物中生物可利用Hg在MeHg的产生过程中具有重要作用,而减少大连湾内汞和有机质的输入将有助于降低沉积物中w（MeHg）.      

武汉城市湖泊表层底泥汞分布、风险评价及影响因素

底泥作为汞重要的"汇"及二次"源"，在湖泊系统汞生物地球化学循环中起到了重要作用。本文以武汉主要城市湖泊为研究对象，探究了表层底泥中总汞（THg）和甲基汞（MeHg）的分布特征、潜在生态风险及主要影响因素。结果表明，武汉15个城市湖泊表层底泥THg平均浓度为152±170 ng/g （24~611 ng/g），与国内其它湖泊系统相比处于较高水平；MeHg浓度为52.0±46.8 pg/g （ND~161.0 pg/g），低于其它湖泊系统。空间分布上，底泥THg浓度呈现由武汉市中心向外逐渐递减的趋势，MeHg含量并未呈现类似THg的分布趋势。潜在生态风险评价（PERI）结果显示，所有采样点位中汞潜在生态风险极高和高风险等级占比均为5.7%，且主要分布在市中心附近，说明武汉市中心附近湖泊底泥汞污染程度较重，而市中心外围湖泊底泥汞生态风险较低。相关性分析结果显示，有机质可能是影响武汉城市湖泊底泥THg分布的重要因素之一，而MeHg主要受控于无机汞的原位甲基化过程。底泥THg浓度-湖泊距市中心距离间显著的负相关关系、THg浓度-湖泊所在区GDP/人均GDP间的显著正相关关系均表明人为活动对武汉城市湖泊汞分布影响明显。     

典型汞污染河流生物膜和沉积物中汞的分布特征

为弄清汞污染历史河流水体、生物膜和沉积物中汞污染现状和潜在风险,本研究选择贵州省清镇市东门桥河为研究对象,采集河流水体、生物膜和沉积物样品,并测定其汞的形态含量。结果表明,东门桥河水体总汞(THg)、溶解态汞(DHg)和颗粒态汞(PHg)的平均含量分别为66.46±51.87 ng/L、10.67±5.15 ng/L和55.79±50.26 ng/L,PHg含量高达72%。生物膜中THg和MeHg的平均含量分别为9.38±12.39 mg/kg、19.58±22.21μg/kg;沉积物中THg和MeHg的平均含量分别为30.89±24.64 mg/kg、21.50±7.20μg/kg。水体和生物膜中汞的季节分布特征为夏季秋季春季。受清淤情况和市政污水排放的影响,随着采样点逐渐远离总排污口,水体汞含量呈现逐渐升高的趋势,而沉积物和生物膜的汞含量呈现出逐渐下降的趋势。     

太湖不同营养水平湖区汞的形态和分布特征

为研究富营养化对太湖汞形态分布特征的影响,于2011年水华暴发期,在太湖不同营养水平湖区(竺山湾、贡湖湾及南太湖)采集水样,测定了水体中THg(总汞)、DHg(溶解态总汞)、RHg(活性汞)、TMeHg(总甲基汞)、DMeHg(溶解态甲基汞)的质量浓度及其分布特征. 结果表明,太湖不同营养水平湖区水体中ρ(THg)和ρ(DHg)无显著差异,ρ(THg)为4.67~12.15 ng/L,ρ(DHg)为2.27~10.36 ng/L. 太湖水体中ρ(RHg)平均值为0.79 ng/L,藻类的生长对水体中ρ(RHg)的分布有显著影响,水体营养水平越高,ρ(RHg)越低. 水体中ρ(TMeHg)和ρ(DMeHg)分别为0.10~0.27和0.09~0.23 ng/L,藻类的吸附及水体中较高的E_h(氧化还原电位)和pH抑制了汞的甲基化,但在富营养化较严重的竺山湾,受藻类生长及水华的影响,水体中ρ(TMeHg)(0.22 ng/L)仍相对较高.      

汞在酸性紫色水稻土的转化与水稻汞富集特征

采用盆栽模拟试验,对汞(Hg)及甲基汞(MeHg)在酸性紫色水稻土中不同水稻生长期的动态变化进行了研究,并分析对比了总汞(THg)和MeHg在水稻体中的富集特征.结果表明:在水稻生长期间,土壤总汞含量变化较小,MeHg含量随时间增加而增加,土壤MeHg/THg值的变化趋势和土壤中MeHg含量变化一致.完熟期THg在水稻中植株的分布状况为:根籽粒茎叶穗壳,MeHg的分布为:籽粒根茎叶穗壳.水稻植株中MeHg/THg均值为24.03%,大于土壤均值3.05%,说明水稻植株中具有较强的MeHg累积能力.在水稻生长周期内,水稻体内MeHg富集系数均值为8.16,远大于THg富集系数的均值2.31,且籽粒中的MeHg富集系数大于根、茎、叶,说明水稻对MeHg的富集能力强于THg,且籽粒更易于富集MeHg.水稻体内的MeHg的转移系数大于THg,且籽粒中MeHg的转移系数大于1,进一步说明MeHg比THg更易在水稻体内转移.     

中国十条主要入海河流河口汞的形态分布特征与入海通量估算

为了解我国河流向海洋汞的输送通量,选取我国沿海10条大型河流的河口作为采样点,采集水体和沉积物,测定水中不同形态汞,包括总汞（THg）、溶解态汞（DHg）、颗粒态汞（PHg）、总氮（TN）、总磷（TP）和溶解有机碳（DOC）等,测定了沉积物THg和甲基汞（MeHg）等.结合河流的径流量,对陆地经河流向海洋汞的输入量进行了粗略的估算.结果显示：我国十条主要入海河流地表水THg含量为2.79~145.15 ng·L^-1,DHg含量为0.61~4.44 ng·L^-1,PHg含量为1.28~143.54 ng·L^-1.PHg约占THg含量的41%~99%,DHg约占THg含量的1%~35%.表层沉积物THg含量为0.02~0.3 mg·kg^-1,MeHg含量为0.04~2.00 μg·kg^-1.MeHg百分含量为0.1%~1.2%.沉积物THg、MeHg和 TOC之间呈显著相关性（p<0.01）.我国主要河流经径流输入THg的入海通量为10.01~29.92 t·a^-1,长江是我国河流向海洋汞输送通量的贡献量最大,约占到我国主要河流入海汞通量的58%~69%.本研究基于实测数据的估算值与前人的估算结果对比,我国主要河流的入海汞通量仅占全球入海汞通量0.2%~15%;对比前人对中国河流向海洋汞的输送通量实测结果以及模型模拟结果显示,实测结果在同一数量级,且实测结果比模拟结果更可靠.     

不同功能区污水中汞的含量、形态和负荷研究

该研究以焦作市5种不同功能区(居民区、商业区、学校、牙科诊所和医院)的污水作为研究对象,分析了其中汞的浓度和形态,进而对不同功能区污水的汞负荷进行了估算。结果显示,牙科诊所污水中的总汞(THg)和甲基汞(MeHg)浓度最高,均值分别为(11.3±10.6)μg/L和(18.17±31.76) ng/L。医院污水样品THg和MeHg浓度均值分别为(324.70±274.22) ng/L和(6.84±3.85) ng/L。居民区、商业区和学校的污水中THg的浓度相差不大,均值分别为(179.15±54.20)、(256.04±123.93)和(156.65±42.63) ng/L;MeHg浓度分别为(2.42±0.71)、(2.67±1.68)和(1.80±0.40) ng/L。所有样品中,溶解态总汞(DTHg)占THg的比例为0.74%～23.37%之间,溶解态甲基泵(DMeHg)占MeHg的比例为23.41%～45.70%,说明污水中的汞主要以颗粒态存在;污水样品MeHg占THg的比例为1.10%～4.48%。牙科诊所的污水中,THg和MeHg的浓度都很高,需要采取有效措施减少牙科污水中汞的排放。以居民区、商业区、学校生活污水汞浓度的均值来估算,全国城镇生活污水的THg负荷为(6.41±1.68)t/a,相当于全国城市污泥THg负荷的(52.54±13.77)%,是城市污水中汞的主要贡献源。以牙科医生的平均THg负荷计算,全国牙科污水的THg负荷为(193.13±198.01) kg/a,对全国城市污泥THg负荷的贡献率约为(1.58±1.62)%;以医院床位的平均THg负荷计算,全国医院污水的THg负荷为(142.53±224.22) kg/a,对全国污泥中THg负荷的贡献率约为(1.17±1.84)%,可见牙科诊所污水和医院污水不是城市污水中汞的主要贡献源。     

三峡库区消落带农业活动对土壤汞变化的影响

针对三峡库区消落带退水期农业生产是否会对库区环境带来不利影响的问题,以分布面积较大、农业活动较为频繁的重庆市开州区渠口镇消落带为研究区域,选择种植水稻、玉米、蔬菜和未农用的草地4类消落带地块为研究对象,调查了不同利用地块表层土壤汞(Hg)的变化特征.结果表明,研究区域内土壤THg、有效态Hg(Hg-wh)和甲基汞(MeHg)平均含量分别为25.80~68.74、0.44~0.88和0.08~0.85 ng·g-1.未耕作土地表层土壤THg、Hg-wh和MeHg含量均高于耕作土地表层土壤,说明耕作扰动能够加速土壤Hg的流失.未耕作土壤与耕作土地表层土壤MeHg含量随着落干时长的增加均呈现先升高后降低的趋势,峰值大约出现在落干后1~2个月内,约为淹水末期的4倍,之后逐渐降低至相对稳定的水平.MeHg占THg比例(%MeHg)也呈现类似规律,峰值出现在落干后1个月左右,降到稳定水平时与淹水末期含量无显著性差异(P0.05).土壤%MeHg与Hg-wh含量呈显著性正相关关系(r=0.642,P0.01),而与THg含量没有显著相关性(P0.05),说明消落带土壤Hg甲基化主要受生物可利用性Hg形态的影响.     

三峡库区消落带沉积物对鱼体富集汞的影响

水体环境中的汞（Hg）容易被鱼体富集.为了研究三峡库区消落带沉积物对鱼体Hg含量的影响,采用不同Hg含量的消落带沉积物进行了为期90 d的模拟淹水实验.结果表明沉积物淹水后,水体总汞（THg）和甲基汞（MeHg）含量显著增加,鱼体肌肉中THg和MeHg含量不断增加,而内脏和头部中THg和MeHg含量前期不断增加,后期则有轻微减小的趋势.肌肉对Hg的富集量大于内脏和头部,后两者的富集量没有显著性差异.与对照组（无沉积物）相比沉积物的存在明显增加了鱼体富集Hg的量,而且当沉积物中Hg含量较高时,鱼体对Hg的富集量也显著增加.鱼体各部位THg和MeHg含量变化曲线高度相似,各部位对MeHg的富集系数（bioaccumulation factors,BCF）在1.93×10⁵~8.89×10⁵之间,对无机Hg的BCF在1.3×10³~12.8×10³之间,表明鱼体所富集的Hg形态上主要为MeHg.鱼体各部位MeHg和THg含量均为极显著相关,线性回归方程表明,在富集Hg的量中,MeHg占THg比例分别为：肌肉80.1%、内脏79.3%、头部66.7%.消落带沉积物再淹水后会发生一定程度的净甲基化现象产生MeHg,由于扩散作用使水体MeHg浓度在一段时间内升高,这导致了鱼体对Hg的富集量增加.因此对三峡库区大面积消落带可能存在的Hg污染风险不可忽视.     

Methylmercury and sulfate-reducing bacteria in mangrove sediments from Jiulong River Estuary, China

Estuaries are important sites for mercury (Hg) methylation, with sulfate-reducing bacteria (SRB) thought to be the main Hg methylators. Distributions of total mercury (THg) and methylmercury (MeHg) in mangrove sediment and sediment core from Jiulong River Estuary Provincial Mangrove Reserve, China were determined and the possible mechanisms of Hg methylation and their controlling factors in mangrove sediments were investigated. Microbiological and geochemical parameters were also determined. Results showed that SRB constitute a small fraction of total bacteria (TB) in both surface sediments and the profile of sediments. The content of THg, MeHg, TB, and SRB were (350 150) ng/g, (0.47 0.11) ng/g, (1.4 1011 4.1 109) cfu/g dry weight (dw), and (5.0 106 2.7 106) cfu/g dw in surficial sediments, respectively, and (240 24) ng/g, (0.30 0.15) ng/g, (1.9 1011 4.2 1010) cfu/g dw, and (1.3 106 2.0 106) cfu/g dw in sediment core, respectively. Results showed that THg, MeHg, TB, MeHg/THg, salinity and total sulfur (TS) increased with depth, but total organic matter (TOM), SRB, and pH decreased with depth. Concentrations of MeHg in sediments showed significant positive correlation with THg, salinity, TS, and MeHg/THg, and significant negative correlation with SRB, TOM, and pH. It was concluded that other microbes, rather than SRB, may also act as main Hg methylators in mangrove sediments.     

Spatial distribution and pollution assessment of mercury in sediments of Lake Taihu, China

Spatial distribution patterns of total mercury (THg) in 36 surficial sediment samples representing five regions of Lake Taihu were assessed using the ArcGis geostatistical analyst module. The pollution levels of THg were also evaluated from the same five lake regions. Concentrations of THg were in a ranged of 23-168 ng/g (mean 55 ng/g) in surfical sediments, which was significantly higher than those established baseline levels of the lake. Results of THg indicated that the northern region exhibited notably higher values, the bay regions showed elevated values relative to open areas, and the lakeside regions were higher than those observed in the central area. Lake Taihu suffered moderate to high Hg pollution, and expressed clear Hg enrichment status according to monomial pollution index I geo and human activity factors. The concentrations of THg in the surficial sediments of Lake Taihu showed moderate-strong variation (coefficient of variation 52%). Geostatistical analysis indicated a weak spatial self-correlation, suggesting the contamination of Hg in Lake Taihu is primarily the result of anthropogenic activities.     

Ant colonization increased total mercury but reduced methylmercury contents in boreal mires, Northeast China

Soil macroinvertebrates as ecosystem engineers play significant, but largely ignored, roles in affecting mercury (Hg) cycle by altering soil physical-chemical properties. Ant is likely expanded into boreal mires with climate warming, however, its impacts on Hg cycle remained poorly understood. We compared total Hg (THg) and methylmercury (MeHg) contents in soils from antmounds (Lasius flavus) and the nearby ambient in a boreal mire in Northeast China. The present work seeks to unravel factors that controlling MeHg levels in case of ant appearance or absence. The average THg was 179 µg/kg in the ant mound and was 106.1 µg/kg in nearby soils, respectively. The average MeHg was 10.9 µg/kg in the ant mound and was 12.9 µg/kg in nearby soils, respectively. The ratios of MeHg to THg (%MeHg) were 7.61% in ant mounds and 16.75% in nearby soils, respectively. Ant colonization caused THg enrichment and MeHg depletion, and this change was obvious in the 10-20 cm depth soil layer where ants mainly inhabited. Spectrometry characteristics of soil dissolved organic matter (DOM) exert a stronger control than microorganisms on MeHg variation in soils. A structural equation model revealed that the molecular weight of DOM inhibited MeHg irrespective of ant presence or absence, while humification conducive to MeHg significantly in ant mound soils. Microorganisms mainly affected Hg methylation by altering the molecular weight and humification of DOM. We propose that the effects of ant colonization on MeHg rested on DOM feature variations caused by microorganisms in boreal mires.     

三门峡水库水体中不同形态汞的分布特征

为了解三门峡水库水体中不同形态汞的分布特征,在丰水期和枯水期对三门峡水库进行采样,分别采用冷原子荧光光谱法(CVAFS)和蒸馏-乙基化衍生-气相色谱-冷原子荧光法(GC-CVAFS)测定水样中总汞、总甲基汞、溶解态总汞和溶解态甲基汞的浓度.结果表明,三门峡水库水体中总汞、溶解态汞和颗粒态汞浓度范围分别为1.65~9.65、0.80~3.16和0.70~7.81 ng·L~(-1),符合国家地表水环境质量标准(GB 3838-2002)一类水汞浓度标准限值;总甲基汞、溶解态甲基汞和颗粒态甲基汞浓度分别为0.05~0.36、0.02~0.14和ND~0.26 ng·L~(-1).三门峡水库水体总汞和甲基汞在季节和空间分布上没有呈现出明显的变化规律.总汞和甲基汞与未受污染的天然水体差别不大,水库未受到明显的汞污染.丰、枯水期沉积物中总汞浓度分别为(92.96±10.65)ng·g~(-1)和(80.06±19.14)ng·g~(-1),甲基汞浓度分别为(0.33±0.14)ng·g~(-1)和(0.50±0.19)ng·g~(-1).较低的甲基汞浓度说明在三门峡水库汞的迁移转化过程中,甲基化作用可能并非主要的过程,这可能与水体底层溶解氧浓度较高以及沉积物中有机质浓度较低有关.     

Distribution characteristics of total mercury and methylmercury in the topsoil and dust of Xiamen, China

The levels and distribution of mercury (Hg) species, including total mercury (THg) and methylmercury (MeHg) in the topsoil and dust collected from twenty sampling stations located in di erent land function areas of Xiamen, China, were investigated. The THg concentrations in topsoil ranged from 0.071 to 1.2 mg/kg, and in dust ranged from of 0.034 to 1.4 mg/kg. For stations where the THg of dust was less than 0.31 mg/kg, THg concentrations in the topsoil were significantly correlated to those in the corresponding dust (r = 0.597, n = 16, P = 0.014). The MeHg concentrations in topsoil were varied between 0.14 and 5.7 g/kg. The ratios of MeHg/THg in the topsoil ranged from 0.069% to 0.74%. The range of MeHg concentration in the dust were 0.092–2.3 g/kg. The ratios of MeHg/THg in the dust were at the same level as those in the topsoil. The MeHg concentrations in both topsoil and dust were linked to corresponding THg concentrations and soil organic matter. Neither THg nor MeHg concentration in the topsoil and dust was obviously linked to the land function.     

Trophic transfer of mercury and methylmercury in an aquatic ecosystem impacted by municipal sewage effluents in Beijing,China

Gaobeidian Lake, located in Beijing, China, serves as a recipient lake for efluents from a large municipal sewage treatment plant (MSTP). In order to evaluate the effects of discharging MSTP efluent on the mercury contamination of the local aquatic ecosystem, sediment cores, water, plankton, fish, and turtle samples were collected from Gaobeidian Lake for mercury speciation analysis. High concentrations of total mercury (T-Hg) were detected in sediment cores (5.24–17.0 μg/g dry weight (dw), average: 10.1 μg/g). The ratio of methylmercury (MeHg) to T-Hg was less than 0.3% in sediments and ranged from 35% to 76% in biota samples. The highest level of T-Hg and MeHg were found in aquatic bryophyte and crucian carp (3673 and 437 ng/g dw, respectively). The relative contents of MeHg were significantly correlated with trophic levels (R2 = 0.5506, p 0.001), which confirmed that MeHg can be bio-transferred and biomagnified via food chain in this aquatic ecosystem.     

Trophic transfer of mercury and methylmercury in an aquatic ecosystem impacted by municipal sewage e uents in Beijing, China

Gaobeidian Lake, located in Beijing, China, serves as a recipient lake for e uents from a large municipal sewage treatment plant (MSTP). In order to evaluate the e ects of discharging MSTP e uent on the mercury contamination of the local aquatic ecosystem, sediment cores, water, plankton, fish, and turtle samples were collected from Gaobeidian Lake for mercury speciation analysis. High concentrations of total mercury (T-Hg) were detected in sediment cores (5.24–17.0 g/g dry weight (dw), average: 10.1 g/g). The ratio of methylmercury (MeHg) to T-Hg was less than 0.3% in sediments and ranged from 35% to 76% in biota samples. The highest level of T-Hg and MeHg were found in aquatic bryophyte and crucian carp (3673 and 437 ng/g dw, respectively). The relative contents of MeHg were significantly correlated with trophic levels (R2 = 0.5506, p < 0.001), which confirmed that MeHg can be bio-transferred and biomagnified via food chain in this aquatic ecosystem.