沉积物中汞的生物可利用性研究进展

沉积物是汞在水体中的主要分布相,同时也被认为是许多水生生物摄取汞的主要途径,本文综述了近年来在沉积物中汞的生物可利用性领域所取得的最新研究进展,包括体外消化液萃取法估测沉积物中汞的生物可利用性、可能影响汞生物可利用性的生物地球化学因素(汞在沉积物中的浓度、沉积物的组成、汞与沉积物的接触时间、汞与沉积物的结合形式,以及沉...     

Mercury removal from coal combustion flue gas by modified fly ash

Fly ash is a potential alternative to activated carbon for mercury adsorption. The effects of physicochemical properties on the mercury adsorption performance of three fly ash samples were investigated. X-ray fluorescence spectroscopy, X-ray photoelectron spectroscopy, and other methods were used to characterize the samples. Results indicate that mercury adsorption on fly ash is primarily physisorption and chemisorption. High specific surface areas and small pore diameters are beneficial to efficient mercury removal. Incompletely burned carbon is also an important factor for the improvement of mercury removal efficiency, in particular. The C-M bond, which is formed by the reaction of C and Ti, Si and other elements, may improve mercury oxidation. The samples modified with CuBr2 , CuCl 2 and FeCl3 showed excellent performance for Hg removal, because the chlorine in metal chlorides acts as an oxidant that promotes the conversion of elemental mercury (Hg0) into its oxidized form (Hg2+). Cu2+ and Fe3+ can also promote Hg 0 oxidation as catalysts. HCl and O2 promote the adsorption of Hg by modified fly ash, whereas SO2 inhibits the Hg adsorption because of competitive adsorption for active sites. Fly ash samples modified with CuBr2 , CuCl2 and FeCl3 are therefore promising materials for controlling mercury emissions.     

硫酸盐对污泥高级厌氧消化过程中甲基汞迁移转化的影响

为研究污泥高级厌氧消化过程中甲基汞的迁移转化特征以及硫酸盐对污泥厌氧消化过程中汞形态迁移转化的影响,本研究以高温热水解污泥的厌氧消化为研究对象,考察了不同硫酸盐投加浓度下污泥厌氧消化过程中甲基汞的迁移转化特征.结果表明,污泥厌氧消化初期(第1～3 d)发生了汞的甲基化作用,平均甲基汞/总汞比例由0.024%(比值范围为0.019%～0.033%)增加到0.038%(比值范围为0.030%～0.048%),甲基汞净增量分别增加了3.97、 6.09、 0.17、 3.71和1.66倍,随后第3～5 d却发生了明显的汞去甲基化作用,甲基汞净增量降低了71.25%(范围为67.42%～75.10%).硫酸盐对厌氧消化初期汞的甲基化有一定的抑制,而厌氧消化后期,硫酸盐对汞甲基化影响并不明显,这与带电基团HgHS~-_2、 HgS_2~(2-)降低了中性汞络合物的生物有效性及铁硫化物、硫化汞等对S~(2-)和生物可利用态汞的固定作用有关.通过冗余分析,汞的甲基化受到多种环境因素的影响,丙酸、异丁酸和异戊酸等有机质和Fe可能促进汞甲基化,而蛋白质和较高的pH值可能是污泥厌氧消化过程中汞甲基化的抑制因子.     

海水养殖底泥中外源汞甲基化及生物响应研究

本文选择沙蚕作为底栖生物,通过模拟海水养殖环境,研究在外源汞（Hg （NO₃）₂）胁迫下,沙蚕对汞（Hg）的甲基化和甲基汞（MeHg）的富集,以及沙蚕的生物应激响应.结果表明,海水养殖区沙蚕一方面自身具有将汞转化为MeHg的能力,同时沙蚕扰动会促进沉积物中Hg的甲基化,沙蚕扰动沉积物中MeHg的含量为无扰动沉积物中的1.93倍.随着外源汞含量和暴露时间的增加,沙蚕对MeHg的富集量逐渐增加,而富集速率逐渐降低.沙蚕体内MeHg富集含量为0.007~0.079mg/kg,占沙蚕体内总汞（THg）含量的31.20%~86.90%.与无机Hg相比,MeHg会对沙蚕造成更大的氧化压力,具有更强的生物毒性.沙蚕的SOD,CAT活性和GSH,MDA含量与暴露时间及含量有显著相关性.当沉积物中外源汞输入含量超过0.5mg/kg,沙蚕抗氧化应激系统将超过防御极限.     

互花米草入侵对滨海盐沼土壤甲基汞的影响

本研究跨越11个纬度选取了4个典型滨海盐沼湿地,通过对比分析互花米草湿地和其他盐沼湿地（没有互花米草的本地种单优或者共优群落湿地）的汞（THg）和甲基汞（MeHg）含量特征及环境因子,探究互花米草入侵对我国滨海盐沼湿地土壤甲基汞的影响.结果表明：（1）4个研究区THg含量高低顺序为闽江口（（115.327±18.220）μg/kg） > 杭州湾（（37.792±3.761）μg/kg） > 黄河三角洲（（27.690±4.359）μg/kg） > 盐城（（8.843±1.688）μg/kg）;MeHg含量为杭州湾（（0.589±0.134）μg/kg） > 黄河三角洲（（0.511±0.059）μg/kg） > 闽江口（（0.361±0.065）μg/kg） > 盐城（（0.191±0.027）μg/kg）.（2）综合4个研究区进行分析发现,互花米草入侵对盐沼湿地土壤MeHg和% MeHg的均没有显著影响,但是互花米草入侵著增加了黄河三角洲的MeHg含量（95.0%）.（3）在两种湿地类型中,% MeHg（甲基化率）和THg均呈现极显著的负相关关系,且二者之间的关系存在一个临界值（20~30μg/kg之间）,当THg小于临界值时,% MeHg与环境因子相关性较弱;当THg大于临界值时,% MeHg与环境因子显著相关.本研究从较大的空间尺度回答了互花米草入侵对滨海盐沼湿地甲基汞特征的影响,为全面评价互花米草入侵对我国滨海地区的影响提供了数据支持,为研究滨海滩涂地区汞的迁移转化提供了依据.     

不同硒化修复剂对稻田汞污染修复效果研究

以亚硒酸钠、蒙脱土等作为材料,对蒙脱土进行硒化改性,将硒负载在经过改性的蒙脱土上制备出汞的钝化剂以降低汞和甲基汞（MeHg）在稻米中的富集.将硒化修复剂与污染土壤混合进行浸泡土试验和盆栽试验,分析土壤和稻米中THg和MeHg,探讨不同硒化修复剂对污染土壤中汞的阻控修复效果,并筛选出最佳修复剂.结果表明,4种修复剂均对污染土壤中汞有明显的钝化阻控作用,可显著降低土壤中可交换态汞和甲基汞,降低稻米中THg和MeHg含量.蒙脱土通过不同方式硒化改性后,使蒙脱土结构性能优化,吸附容量增加,并能使硒稳固在蒙脱土上,达到更好的钝化修复效果.硒化壳聚糖改性蒙脱土、亚硒酸钠改性蒙脱土、硒化纤维素改性蒙脱土、硒粉改性蒙脱土4种修复剂稻米THg的降低率依次为81.86%、79.74%、65.69%、61.78%,MeHg降低率依次为89.62%、83.91%、72.93%、63.01%.相比较而言,亚硒酸钠改性蒙脱土修复效果稍低于硒化壳聚糖改性蒙脱土,但其改性方法简单,成本低,更有利于修复剂的推广应用.     

海螺沟冰川融水径流中汞与悬浮颗粒物的季节变化特征及其关系研究

为研究冰川融水径流中汞与悬浮颗粒物的变化及其相关关系,于2019年6月～2020年9月在青藏高原东南缘海螺沟冰川融水径流进行为期一年的连续定点采样,测试了样品中汞形态含量和悬浮颗粒物的数量、含量及粒径特征。分析表明,总汞的平均含量为6.96～10.78 ng/L,其中颗粒态汞为4.54～9.14 ng/L,溶解态汞为1.53～2.42 ng/L,与青藏高原及世界其他偏远地区河流汞含量相当。各形态汞与悬浮颗粒物不同特征在不同季节的相关关系差异显著,总汞和颗粒态汞含量与总悬浮颗粒物含量和数量在夏季消融盛期具有突出且一致的正相关关系,但在秋冬季并未显示出正相关,表明前人揭示的冰川补给河流中颗粒物控制汞含量变化的结论具有季节局限性。冰川径流中的汞受水文过程和汞的来源及其在水体中的转化等多因素影响,汞形态含量与悬浮颗粒物不同物理特征在不同季节的差异性可能反映了不同季节汞的来源和传输机制的差异。     

Vertical distribution characteristics of soil mercury and its formation mechanism in permafrost regions: A case study of the Qinghai-Tibetan Plateau

Continuing permafrost degradation is increasing the risk of mercury(Hg) exposure in the permafrost regions on the Qinghai-Tibetan Plateau(QTP), but related studies are still limited, especially the ones on the detailed Hg migration processes in permafrost. The vertical distribution characteristics of soil Hg were investigated in three ecosystems in the Beiluhe area on the QTP, and its influencing factors and formation mechanism were investigated. The results indicate that the total soil mercury(...     

Improved atmospheric mercury simulation using updated gas-particle partition and organic aerosol concentrations

The gaseous or particulate forms of divalent mercury (Hg^II) significantly impact the spatial distribution of atmospheric mercury concentration and deposition flux (FLX). In the new nested-grid GEOS-Chem model, we try to modify the Hg^II gas-particle partitioning relationship with synchronous and hourly observations at four sites in China. Observations of gaseous oxidized Hg (GOM), particulate-bound Hg (PBM), and PM_2.5 were used to derive an empirical gas-particle partitioning coefficient as a function of temperature (T) and organic aerosol (OA) concentrations under different relative humidity (RH). Results showed that with increasing RH, the dominant process of Hg^II gas-particle partitioning changed from physical adsorption to chemical desorption. And the dominant factor of Hg^II gas-particle partitioning changed from T to OA concentrations. We thus improved the simulated OA concentration field by introducing intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emission inventory into the model framework and refining the volatile distributions of I/SVOCs according to new filed tests in the recent literatures. Finally, normalized mean biases (NMBs) of monthly gaseous element mercury (GEM), GOM, PBM, WFLX were reduced from −33%–29%, 95%–300%, 64%–261%, 117%–122% to −13%–0%, −20%–80%, −31%–50%, −17%–23%. The improved model explains 69%–98% of the observed atmospheric Hg decrease during 2013–2020 and can serve as a useful tool to evaluate the effectiveness of the Minamata Convention on Mercury.