大气汞源解析受体模型研究进展

大气汞循环演化对全球汞的生物地球化学循环起着极其重要的作用。人为活动(化石燃料燃烧、水泥生产、氯碱制造以及金属冶炼与加工等)已成为大气汞的重要来源。在一定条件下,大气中的汞会发生干湿沉降而对某一局部环境——受体产生很大的影响。大气汞沉降在城市和工业区呈现出很强的空间梯度现象,排放源附近的汞沉降量明显较强。利用对受体的研究开展大气汞的源解析工作,是大气汞研究的一个重要领域。本文综述了污染物源解析的受体模型的研究及应用,介绍了化学质量平衡法、因子分析法、正交矩阵因子分解法、多元线性回归法等方法,概括了源解析在大气汞方面的应用成果,对我国区域大气汞源解析受体模型的建立及应用进行了探讨。     

地表自然过程排汞研究进展及展望

地表自然过程排汞包括了自然源排汞过程和先前排放的汞沉降到地表后的再排放过程.已有证据显示,地表自然过程向大气的排汞量可能远大于人为活动直接向大气的排汞量.准确确定自然过程汞的释放通量,不仅对正确评价目前减少人为活动向大气排汞对全球环境汞污染的影响程度具有重要的意义,而且可为全球大气汞的减排政策的制定提供重要科学理论依据.本综述通过对国内外地表自然排放源相关文献的调研分析发现:由于缺少可靠的观测技术、对地表与大气间汞交换过程和机理的准确认识及大气汞沉降对地表自然排汞过程影响的认识还不清楚,因此目前还难以准确估算地表自然过程向大气的排汞量.近年来,随着技术手段的进步,已具备了开展地表自然排汞及先前排汞沉降后的再释放过程、机理和通量研究的可行性.地表自然过程排汞的研究将是汞的生物地球化学循环演化研究领域的前沿之一.     

我国自然源汞排放研究进展

由于特殊的物理化学性质,汞是唯一主要以气态单质形式存在于大气的重金属污染物,可通过大气环流进行全球性的传输。大气汞主要来自于人为活动和自然过程的汞排放。建立和优化全球和区域大气汞排放清单对研究全球大气汞的迁移转化规律及其环境健康效应具有重要意义。由于影响因素较为复杂,目前国内外自然源清单研究与人为源清单研究相比较为滞后。我国约十分之一的国土面积位于环太平洋汞矿化带上,且我国主要自然源汞排放通量与欧洲和北美同类型地区相比偏高。近些年来,国内研究人员在自然源汞排放研究领域开展了大量的研究工作,为建议和优化我国的自然源汞排放清单提供了重要的科学依据。本文总结了近年来我国自然源汞排放的研究进展,分析水体、土壤和植被等自然源汞排放通量分布规律、内在机理和影响因素;同时对我国自然源汞排放存在的不足及未来需要开展的工作进行了展望。     

腐殖质、硫、氯化钠对水稻积累汞的影响试验研究

汞是环境中主要重金属污染物之一。国内外在研究汞在水生环境的迁移转化规律及其基质方面进行了大量的工作,但汞在陆生环境中的迁移转化,尤其是土壤—植物系统中影响汞吸收的机制方面研究得较少。近年来,国外对影响土壤吸收汞的机制的研究工作,认为土壤酸碱度、氧化还原电位是影响土壤、生物吸收重金属的主要因素,环境中无机配位体和有机     

汞在SPAC-人体系统中的转递及主要影响因素

汞（Hg）是环境中一种具有高度毒性的重金属元素,且具有较高挥发性,因而作为一种全球性的污染物而备受关注。汞在SPAC系统中的迁移转化,是全球汞循环的重要环节,与人类的建康密切相关。汞通过食物链进入人体并在体内蓄积受多种因素影响,主要包括3个方面：土壤性质（如土壤汞含量、pH、有机质、粘土矿物等）,植物特性（植物类型、种类和生育期等）,大气状况（如光照强度、气温和大气湿度等）。此外,锌、硒和抗氧化剂等的存在也有较大影响。综述了汞在SPAC-人体系统中的迁移积累及其调控机理。     

大气氮沉降的基本特征与监测方法

大气氮沉降主要以干湿沉降两种形式将有机和无机形态的氮带入生态系统,是氮素生物地球化学循环的重要环节之一.近年来人类活动的加强,使得大量活性氮素进入大气,高排放量导致氮沉降通量急剧上升,引起一系列的环境风险,因此,对大气氮沉降的研究也越来越受到关注.本文总结了大气氮沉降的组分、过程、时空变异及生态效应,归纳了目前采用的干湿沉降的监测手段、临界负荷计算方法及污染物来源解析方法等,展望了氮沉降研究的发展趋势.     

南极海-陆界面营养物质流动和磷循环

南极大陆气候严寒、营养贫瘠,企鹅、海豹等生物能传递海洋中的营养物质到陆地,这些营养物质是维系南极无冰区生态系统的基础.本文首先阐述了海洋向南极无冰区输入营养物质的方式,重点介绍了生物方式输入的营养物质对无冰区生态系统组成、结构和功能的影响,以及无冰区向近海输入营养物质的方式及其影响.然后,以西南极法尔兹半岛为例,对企鹅、海豹传输的营养物质磷在陆地、淡水生态系统中的记录进行了分析,讨论了南极近海磷的生物地球化学循环及其机理,估算了磷循环通量.结果表明,南极阿德雷岛磷的外来营养源包括物理输入、生物输入和大气沉降输入3种,其中,生物输入(企鹅粪)占94.34％ ～ 99.74％,在近海磷循环中起着关键作用.     

生物炭对污染物的土壤环境行为影响研究进展

近年来,生物炭已成为农业、生态修复和环境保护领域的研究热点。一般认为,生物炭具有改善土壤质量、增加土壤碳汇、减少大气CO2浓度以及修复污染环境等功能。大量的生物炭施用到土壤后会改变土壤性质,影响重金属和有机污染物在土壤中的环境行为以及它们在环境中的归趋。本文就生物炭对土壤中重金属的吸附-解吸、在土壤中的形态转化、在土壤-植物系统中迁移行为、对有机污染物的吸附挥发及生物有效性进行了概述;在此基础上,扼要分析了当前生物炭应用存在的环境风险等问题,并从生物炭在土壤中的迁移转化及其归趋、生物炭的长期环境效应以及生物炭应用方向等方面进行了展望。     

生物土壤结皮对全球气候变化的响应

生物土壤结皮在干旱、半干旱区和极地、亚极地区等脆弱生态区广泛存在,生物土壤结皮对脆弱生态系统的稳定、碳氮循环和生态平衡等具有重要的生态意义.概述了脆弱生态区生物结皮的碳氮循环与气候变化关系,综合分析了脆弱生态区生物结皮对气候变暖、降水变化和UV-B增加的响应.分析认为应该加强区域尺度下干旱与半旱区生物结皮对气候变化响应研究.     

基于BIOLOG技术分析氮沉降和降水对土壤微生物功能多样性的影响

土壤微生物是有机物分解和养分循环的主要介质,因此在维持土壤的功能多样性和持续性方面发挥着关键作用。气候变化驱动因素会影响土壤微生物的生理活动,引起其群落结构和功能多样性的改变,并对生物地球化学循环和气候―生态系统反馈产生连锁效应,其中氮沉降和降水是全球气候变化的研究热点。土壤氮(N)的有效性有可能通过改变微生物的群落组成以调节微生物对降水变化的响应,但目前关于N沉降和降水及其交互作用对土壤微生物群落功能多样性的影响机制仍不清楚。为了准确预测未来气候条件下生态系统的功能状况,需要更好地了解土壤微生物对环境变化的响应。基于BIOLOG技术综述了氮沉降和降水变化及其交互作用对土壤微生物功能多样性影响的相关研究进展,可以为进一步研究全球气候变化背景下地下生态学的发展提供参考。另外,分析阐述了当前工作中存在的一些主要瓶颈,并对未来的研究热点进行了探讨和展望。     

Application of tree rings [dendrochemistry] for detecting historical trends in air Hg concentrations across multiple scales

Tree rings are a useful long term monitor of climate change indicators and certain atmospheric constituents. Since we have no long-term historical record of air mercury (Hg) concentrations, and previous research demonstrates atmospheric uptake of Hg into vegetative biomass, we hypothesized that tree rings would be a useful archive for monitoring changes in local, regional, and global air Hg concentrations. We developed and tested a method for measurement of Hg in tree rings, and then investigated our hypothesis using species within the genus Pinus. Mercury concentrations declined along a coast-to-interior (California-to-Nevada, USA) gradient with highest mean concentrations (5.7 ng/g) at the coast, and lowest (<1.2 ng/g) at inland locations. Tree ring Hg concentrations recorded the impact of local sources and indicate increasing global concentrations over time. The data also indicate that concentrations are higher in areas impacted by marine air, and this suggests that the atmospheric chemistry is influencing assimilation. Future research should address species- and age-specific variation in the sensitivity of tree-ring samples as proxy data for atmospheric Hg concentrations. Tree rings show great potential as passive recorders of atmospheric Hg for long time periods (centuries to millennia) at time steps of ≤5 years.     

Increased mercury in forest soils under elevated carbon dioxide

Fossil fuel combustion is the primary anthropogenic source of both CO₂ and Hg to the atmosphere. On a global scale, most Hg that enters ecosystems is derived from atmospheric Hg that deposits onto the land surface. Increasing concentrations of atmospheric CO₂ may affect Hg deposition to terrestrial systems and storage in soils through CO₂-mediated changes in plant and soil properties. We show, using free-air CO₂ enrichment (FACE) experiments, that soil Hg concentrations are almost 30% greater under elevated atmospheric CO₂ in two temperate forests. There were no direct CO₂ effects, however, on litterfall, throughfall or stemflow Hg inputs. Soil Hg was positively correlated with percent soil organic matter (SOM), suggesting that CO₂-mediated changes in SOM have influenced soil Hg concentrations. Through its impacts on SOM, elevated atmospheric CO₂ may increase the Hg storage capacity of soils and modulate the movement of Hg through the biosphere. Such effects of rising CO₂, ones that transcend the typically studied effects on C and nutrient cycling, are an important next phase for research on global environmental change.     

Atmospheric mercury pollution due to losses of terrestrial carbon pools?

Plants accumulate significant amounts of atmospheric mercury (Hg) in aboveground biomass, likely sequestering over 1,000 Mg of atmospheric Hg every year. This large mercury uptake could be strong enough to affect tropospheric Hg levels and might be partially responsible for seasonal variations in atmospheric Hg observed at Mace Head, Ireland. The fluctuations of Hg concentrations coincide temporally with the annual oscillation of carbon dioxide (CO₂) in the Northern Hemisphere, which is a result of seasonal growth of vegetation. Therefore, declining Hg concentrations in spring and summer may be attributed in part to plant uptake of atmospheric Hg. Further, the increase of Hg concentrations during non-active vegetation periods might partially be due to plant-derived Hg emitting back to the atmosphere during carbon mineralization. The implications of these propositions are that past and future changes in biomass productivity and organic carbon pools may have had—and may continue to have—significant effects on atmospheric Hg levels. Specifically, large losses in soil and biomass carbon pools in the last 150 years could have contributed significantly to observed increases in atmospheric Hg pollution. The roles of vegetation and terrestrial carbon pools should receive detailed consideration on how they might attenuate or exacerbate atmospheric Hg pollution.     

Emissions from Pre-Hispanic Metallurgy in the South American Atmosphere

Metallurgical activities have been undertaken in northern South America (NSA) for millennia. However, it is still unknown how far atmospheric emissions from these activities have been transported. Since the timing of metallurgical activities is currently estimated from scarce archaeological discoveries, the availability of reliable and continuous records to refine the timing of past metal deposition in South America is essential, as it provides an alternative to discontinuous archives, as well as evidence for global trace metal transport. We show in a peat record from Tierra del Fuego that anthropogenic metals likely have been emitted into the atmosphere and transported from NSA to southern South America (SSA) over the last 4200 yrs. These findings are supported by modern time back-trajectories from NSA to SSA. We further show that apparent anthropogenic Cu and Sb emissions predate any archaeological evidence for metallurgical activities. Lead and Sn were also emitted into the atmosphere as by-products of Inca and Spanish metallurgy, whereas local coal-gold rushes and the industrial revolution contributed to local contamination. We suggest that the onset of pre-Hispanic metallurgical activities is earlier than previously reported from archaeological records and that atmospheric emissions of metals were transported from NSA to SSA.     

Modeling and Mapping of Atmospheric Mercury Deposition in Adirondack Park,New York

The Adirondacks of New York State, USA is a region that is sensitive to atmospheric mercury (Hg) deposition. In this study, we estimated atmospheric Hg deposition to the Adirondacks using a new scheme that combined numerical modeling and limited experimental data. The majority of the land cover in the Adirondacks is forested with 47% of the total area deciduous, 20% coniferous and 10% mixed. We used litterfall plus throughfall deposition as the total atmospheric Hg deposition to coniferous and deciduous forests during the leaf-on period, and wet Hg deposition plus modeled atmospheric dry Hg deposition as the total Hg deposition to the deciduous forest during the leaf-off period and for the non-forested areas year-around. To estimate atmospheric dry Hg deposition we used the Big Leaf model. The average atmospheric Hg deposition to the Adirondacks was estimated as 17.4 g m yr with a range of −3.7–46.0 g m yr. Atmospheric Hg dry deposition (370 kg yr) was found to be more important than wet deposition (210 kg yr) to the entire Adirondacks (2.4 million ha). The spatial pattern showed a large variation in atmospheric Hg deposition with scattered areas in the eastern Adirondacks having total Hg deposition greater than 30 μg m⁻² yr⁻¹, while the southwestern and the northern areas received Hg deposition ranging from 25–30 μg m⁻² yr⁻¹.     

Effects of organic solvents on the high performance liquid chromatographic analysis of the cyanobacterial toxin cylindrospermopsin and its recovery from environmental eutrophic waters by solid phase extraction

An Escherichia coli strain was generated by fusion of a merA-deleted broad-spectrum mer operon from Pseudomonas K-62 with a bacterial polyphosphate kinase gene (ppk) from Klebsiella aerogenes in vector pUC119. A large amount of the ppk-specified polyphosphate was identified in the mercury-induced bacterium with the fusion plasmid designated pMKB18 but not in the cells without mercury induction. These results suggest that the synthesis of polyphosphate as well as the expression of the mer genes is mercury-inducible and regulated by merR. The E. coli strain with pMKB18 was more resistant to both Hg2+ and C6H5Hg+ than its isogenic strain with cloning vector pUC119. The recombinant strain accumulated more mercury from Hg2+- and C6H5Hg+-contaminated medium. Hg2+ transported into the cytoplasm appeared to be bound by chelation with the polyphosphate produced by the recombinant cells. The transported phenylmercury was degraded to Hg2+ before the chelation since polyphosphate did not directly chelate with C6H5Hg+. These results indicate that polyphosphate is capable of reducing the cytotoxicity of the transported Hg2+ probably via chelation between polyphosphate and Hg2+.     

Concentration and risk assessments of mercury along the elevation gradient in soils of Langtang Himalayas,Nepal

The fragile Himalayan region could be regarded as the sink for various pollutants transported from urbanized and polluted areas of South Asia. Therefore, in order to understand the concentrations, spatial distribution, pollution, and risk assessments of toxic heavy metal, mercury (Hg), surface soil samples were taken from the central Himalayas in the Langtang region. The average THg concentration in the Langtang Himalayas was 35.75 ± 24.41(ngg^?1), which is comparable to the Tibetan top soil values and slightly lower than world average soil values. In addition, an inverse relationship of THg with elevation were observed (i.e. decrease in concentration with increase in elevation) in the Langtang Himalayan soils. Meanwhile, THg concentrations and TOC% were significantly positively correlated at both the depths (0–10 and 10–20 cm), inferring the sorption capacity of organic carbon for Hg. The results of the geo-accumulation index (I_geo), enrichment factor (EF), and pollution index (PI) indicated limited or no pollution by Hg in the Himalayan soils. Further, surface soils had a low potential ecological risk in the region. Therefore, the Hg value from this study could be used for the further evaluation and calculation of I_geo, EF, and PI for water, soil, and aerosol in the Himalayan region as background reference value. However, Hg pollution from long-range transport and atmospheric deposition (wet/dry) in future could not be ignored in the Himalayan region.     

Phytoremediation of Mercury- and Methylmercury-Polluted Soils Using Genetically Engineered Plants

Inorganic mercury in contaminated soils and sediments is relatively immobile, though biological and chemical processes can transform it to more toxic and bioavailable methylmercury. Methylmercury is neurotoxic to vertebrates and is biomagnified in animal tissues as it is passed from prey to predator. Traditional remediation strategies for mercury contaminated soils are expensive and site-destructive. As an alternative we propose the use of transgenic aquatic, salt marsh, and upland plants to remove available inorganic mercury and methylmercury from contaminated soils and sediments. Plants engineered with a modified bacterial mercuric reductase gene, merA, are capable of converting Hg(II) taken up by roots to the much less toxic Hg(0), which is volatilized from the plant. Plants engineered to express the bacterial organo-mercurial lyase gene, merB, are capable of converting methylmercury taken up by plant roots into sulfhydryl-bound Hg(II). Plants expressing both genes are capable of converting ionic mercury and methylmercury to volatile Hg(0) which is released into an enormous global atmospheric Hg(0) pool. To assess the phytoremediation capability of plants containing the merA gene, a variety of assays were carried out with the model plants Arabidopsis thaliana, and tobacco (Nicotiana tabacum).     

The chemistry and transport of mercury in a small wetland in the Adirondack region of New York, USA

The biogeochemistry of Hg was evaluated in a small wetland in the Adirondack region of New York. Concentrations of total Hg (Hg_T) in streamwater draining the wetland showed little temporal variation. The annual areal watershed flux of Hg_T (2.2 µg/m²-yr) was considerably smaller than regional inputs of atmospheric deposition of Hg_T, indicating that the terrestrial environment is a net sink for atmospheric deposition of Hg_T. Drainage inputs of Hg_T were conservatively transported through the beaver impoundment. The annual flux of total methyl mercury (CH₃Hg⁺ _T was greater than literature values of atmospheric deposition suggesting that the watershed is a net source of CH₃Hg⁺ _T . Stream concentrations of CH₃Hg⁺ _T increased during low-flow summer conditions in a riparian wetland, and particularly at the outlet of the beaver impoundment. Net production of CH₃Hg⁺ _T occurred in the beaver impoundment (0.45 µg/m²-yr). Rates of net methylation for the beaver impoundment were comparable to values reported in the literature for wetlands.     

Reduction of Hg(II) to Hg(0) by Biogenic Magnetite from two Magnetotactic Bacteria

Understanding the biogeochemical cycle of the highly toxic element mercury (Hg) is necessary to predict its fate and transport. In this study, we determined that biogenic magnetite isolated from Magnetospirillum gryphiswaldense MSR-1 and Magnetospirillum magnetotacticum MS-1 was capable of reducing inorganic mercury [Hg(II)] to elemental mercury [Hg(0)]. These two magnetotactic bacteria (MTB) lacked mercuric resistance operons in the genomes. However, they revealed high resistance to Hg(II) under atmospheric conditions and an even higher resistance under microaerobic conditions (1% O₂ and 99% N₂). Neither strain reduced Hg(II) to Hg(0) under atmospheric conditions. However, a slow rate (0.05–0.21 µM·d^?1) of Hg(II) loss occurred from late log phase to stationary phase in two MTBs' culture media under microaerobic conditions. Increased Hg(II) entered both cells under microaerobic conditions relative to atmospheric conditions. The majority of Hg(II) was still blocked by the cell membrane. Hg(II) reduction was more effective when biogenic magnetite was extracted out, with or without the magnetosome membrane envelope. When magnetosome membrane was present, 8.55–13.53% of 250 nM Hg(II) was reduced to Hg(0) by 250 mg/L biogenic magnetite suspension within 2 hours. This ratio increased to 55.07–64.70% while magnetosome membrane was removed. We concluded that two MTBs contributed to the reduction of Hg(II) to Hg(0) at a slow rate in vivo. Such reduction was more favorable to occur when biogenic magnetite is released from dead cells. It proposed a new biotic pathway for the formation of Hg(0) in aquatic systems.