南海游泳动物重金属含量特征及风险评价

以2019年夏季采自南海的11种游泳动物为研究对象,测定分析其体内重金属（Cu、Pb、Zn、Cd、Cr、As和Hg）的含量,并评估了上述重金属的污染状况和健康风险。结果显示,7种重金属在生物体中的含量,均符合国内相关污染评价标准。单因子污染指数均值依次为Zn>Cr>As>Hg>Pb>Cd>Cu,虽然个别物种的部分元素达到轻度或中度污染水平,但生物体内7种重金属的综合污染评价均属于无污染状态。健康风险评估结果表明,其膳食暴露风险、非致癌与致癌风险都较低。研究结果表明,南海夏季游泳动物体内重金属含量较低,几乎不存在人类食用健康风险。     

Phosphorus removal from sediments by Potamogeton crispus: New high-resolution in-situ evidence for rhizosphere assimilation and oxidization-induced retention

Macrophytes are usually chosen for phytoremediation tools to remove P in eutrophic aquatic ecosystems, but the lack of test methods hinders the understanding of removal mechanism and application. In this study, we used the novel technologies combined of Diffusive gradients in thin films (DGT), Planar optode (PO), and Non-invasive micro-test technology (NMT) to explore P dynamics in water-sediment continuum and rhizosphere of Potamogeton crispus over time. Results of the high-resolution in situ measurement showed that labile P(LP_DGT) fluxes at the surficial sediment significantly decreased from approximate 120, 140, and 200 pg/ (cm²?sec) via 30 days incubation period to 17, 40, and 56 pg/(cm²?sec) via that of 15 days. Obvious synchronous increase of LP_DGT was not detected in overlying water, suggesting the intense assimilation of dissolve reactive P via root over time. PO measurement indicated that O₂ concentration around the rhizosphere remarkably increased and radially diffused into deeper sediment until 100% saturation along with the root stretch downwards. NMT detection of roots showed the obvious O₂ inflow into root tissue with the uppermost flux of 30 pmol/(cm²?sec) from surroundings via aerenchyma on different treatment conditions. Different from previous reports, gradually saturating O₂ concentrations around the rhizosphere was principally driven by O₂ penetration through interspace attributing to root stretch downward rather than root O₂ leakage. Increased O₂ concentrations in deep sediment over time finally induced the oxidization of labile Fe(II) into Fe(III) bound P and local P immobilization.     

Assessing the factors impacting the bioaccessibility of mercury (Hg) in rice consumption by an in-vitro method

Mercury (Hg) in rice is drawing mounting concern since methylmercury (MeHg) was found capable of accumulating in rice. In-vitro bioaccessibility is a feasible and reliable method to assess the health effects of Hg in rice and has been utilized in a number of studies. This study was done to investigate the impact of cultivar, planting location, and cooking on the total mercury (THg) and MeHg bioaccessibility of rice, for which multiple statistical analysis methods were used to analyze the significance of their effects. The THg concentrations of rice samples taken from non-Hg contaminated areas of China were all below 15 ng/g and their MeHg concentrations were below 2 ng/g. Cooking could significantly reduce the MeHg bioaccessibility of rice because the MeHg was mainly combined with protein and the protein will be denatured during the cooking process, and then the denatured MeHg is difficult to be dissolved into the liquid phase. Indica- and japonica-type rice cultivars did not show significant differentiation in either the concentration of Hg or its bioaccessibility. However, the glutinous rice type differed significantly from the above rice types, and it showed greater bioaccessibility of THg and MeHg due to its distinct protein contents and starch properties. Planting location can affect the Hg concentration in rice and THg bioaccessibility but has a limited impact on MeHg bioaccessibility. Based on these results, two macro factors (rice cultivar, planting location) are presumed to impact Hg bioaccessibility by how they affect micro factors (i.e., Hg forms).     

Influence of dissolved organic matter on methylmercury transformation during aerobic composting of municipal sewage sludge under different C/N ratios

Current knowledge about the transformation of total mercury and methylmercury (MeHg) in aerobic composting process is limited. In this study, the composition and transformation of mercury and dissovled organic matter (DOM) in aerobic composting process of municipal sewage sludge were were comprehensively characterized, and the differences among the three C/N ratio (20, 26 and 30) were investigated. The main form of mercury in C/N 20 and 26 was organo-chelated Hg (F3, 46%-60%); while the main form of mercury in C/N 30 was mercuric sulfide (F5, 64%-70%). The main component of DOM in C/N 20 and 26 were tyrosine-like substance (C1, 53%-76%) while the main fractions in C/N 30 were tyrosine-like substance (C1, 28%-37%) and fulvic-like substance (C2, 17%-39%). The mercury and DOM varied significantly during the 9 days composting process. Compared to C/N 20 and 26, C/N 30 produced the less MeHg after aerobic composting process, with values of 658% (C/N 20), 1400% (C/N 26) and 139% (C/N 30) of the initial, respectively. Meanwhile, C/N 30 produced the best compost showed greater degree of DOM molecular condensation and humification. Hg fraction had been altered by DOM, as indicated by a significant correlation between mercury species and DOM components. Notably, C/N 30 should be used as an appropriate C/N ratio to control the methylation processes of mercury and degration of DOM.     

Sulfur-driven methylmercury production in paddies continues following soil oxidation

Methylmercury (MeHg) production in paddy soils and its accumulation in rice raise global concerns since rice consumption has been identified as an important pathway of human exposure to MeHg. Sulfur (S) amendment via fertilization has been reported to facilitate Hg methylation in paddy soils under anaerobic conditions, while the dynamic of S-amendment induced MeHg production in soils with increasing redox potential remains unclear. This critical gap hinders a comprehensive understanding of Hg biogeochemistry in rice paddy system which is characterized by the fluctuation of redox potential. Here, we conducted soil incubation experiments to explore MeHg production in slow-oxidizing paddy soils amended with different species of S and doses of sulfate. Results show that the elevated redox potential (1) increased MeHg concentrations by 10.9%−35.2%, which were mainly attributed to the re-oxidation of other S species to sulfate and thus the elevated abundance of sulfate-reducing bacteria, and (2) increased MeHg phytoavailability by up to 75% due to the reductions in acid volatile sulfide (AVS) that strongly binds MeHg in soils. Results obtained from this study call for attention to the increased MeHg production and phytoavailability in paddy soils under elevated redox potentials due to water management, which might aggravate the MeHg production induced by S fertilization and thus enhance MeHg accumulation in rice.     

Understanding the risks of mercury sulfide nanoparticles in the environment: Formation, presence, and environmental behaviors

Mercury (Hg) could be microbially methylated to the bioaccumulative neurotoxin methylmercury (MeHg), raising health concerns. Understanding the methylation of various Hg species is thus critical in predicting the MeHg risk. Among the known Hg species, mercury sulfide (HgS) is the largest Hg reservoir in the lithosphere and has long been considered to be highly inert. However, with advances in the analytical methods of nanoparticles, HgS nanoparticles (HgS NPs) have recently been detected in various environmental matrices or organisms. Furthermore, pioneering laboratory studies have reported the high bioavailability of HgS NPs. The formation, presence, and transformation (e.g., methylation) of HgS NPs are intricately related to several environmental factors, especially dissolved organic matter (DOM). The complexity of the behavior of HgS NPs and the heterogeneity of DOM prevent us from comprehensively understanding and predicting the risk of HgS NPs. To reveal the role of HgS NPs in Hg biogeochemical cycling, research needs should focus on the following aspects: the formation pathways, the presence, and the environmental behaviors of HgS NPs impacted by the dominant influential factor of DOM. We thus summarized the latest progress in these aspects and proposed future research priorities, e.g., developing the detection techniques of HgS NPs and probing HgS NPs in various matrices, further exploring the interactions between DOM and HgS NPs. Besides, as most of the previous studies were conducted in laboratories, our current knowledge should be further refreshed through field observations, which would help to gain better insights into predicting the Hg risks in natural environment.     

Formation of sulfur oxide groups by SO2 and their roles in mercury adsorption on carbon-based materials

The presence of SO₂ display significant effect on the mercury (Hg) adsorption ability of carbon-based sorbent. Yet the adsorption and oxidation of SO₂ on carbon with oxygen group, as well as the roles of different sulfur oxide groups in Hg adsorption have heretofore been unclear. The formation of sulfur oxide groups by SO₂ and their effects on Hg adsorption on carbon was detailed examined by the density functional theory. The results show that SO₂ can be oxidized into SO₃ by oxygen group on carbon surface. Both C-SO₂ and C-SO₃ can improve Hg adsorption on carbon site, while the promotive effect of C-SO₂ is stronger than C-SO₃. Electron density difference analyses reveal that sulfur oxide groups enhance the charge transfer ability of surface unsaturated carbon atom, thereby improving Hg adsorption. The experimental results confirm that surface active groups formed by SO₂ adsorption is more active for Hg adsorption than the groups generated by SO₃.     

Mercury release behaviors of Guizhou bituminous coal during co-pyrolysis: Influence of chlorella

Co-pyrolysis of coal and seaweed can not only effectively decrease the carbon footprint but also improve the quality and output of coal pyrolysis products, however, the influence of seaweed on thermal releasing behaviors of mercury during co-pyrolysis process are still unclear. In this work, the chlorella and Guizhou bituminous coal were mixed and used to reveal the mercury release behavior during co-pyrolysis by the temperature programmed pyrolysis experiments, thermogravimetric and differential thermogravimetric analysis (TG-DTG) and thermogravimetry-mass spectrometry (TG-MS) methods, offering a sufficient explanation on the control technology of mercury pollutants in co-pyrolysis. The results exhibited that a large amount of reducing gases such as CO, H₂ and H₂O were generated in chlorella at the temperature range of 100-500°C, which was favorable for the transformation from oxidized mercury to elemental mercury, thus remarkably increased the release of elemental mercury in the raw coal sample. The mixed chlorella also significantly lowered the decomposition temperature range (from 400-600 to 300-400°C) of pyrite-bound mercury and decreased the decomposition temperatures of the pyrite-bound mercury species. Additionally, in the co-pyrolysis about 91.82% of mercury was released into the gas phase below 400°C and was 13.77% higher than that of in individual pyrolysis of coal.     

SCR气氛下Ce-W/TiO2催化剂的脱硝协同脱汞特性

在固定床反应器上研究了反应温度和烟气组分对Ce-W/TiO₂（物质的量比Ce：W=2：1）催化剂脱硝协同脱汞活性的影响.结果表明：反应温度对该催化剂的脱硝脱汞效率影响显著,在280~400℃温度区间,脱硝效率随温度升高而升高,而脱汞效率在温度为280℃与360℃的条件下较高,360℃时兼具最好的脱硝与脱汞效率.在SCR气氛中,HCl对Hg⁰的氧化脱除有极大的促进作用,低浓度的HCl也有利于脱硝效率的提高,但HCl浓度过高对NO的脱除有抑制作用;SO₂的存在对脱硝过程可起到促进作用,对Hg⁰的氧化有抑制作用.利用BET,XRD,SEM,TPD,XRF,NH3-TPD等分析手段对反应前后催化剂进行表征,结果表明：Ce-W/TiO₂无微孔结构,活性组分CeO₂和WO₃以高度分散的形式分布于载体表面.280℃条件下部分Hg以HgCl₂的形式吸附于反应后催化剂表面,随着反应温度的升高催化剂表面吸附态的汞急剧降低.SCR气氛中的HCl与SO₂会影响催化剂表面酸性,同时增加Cl和S元素含量,进而影响该催化剂的脱硝与脱汞效率.     

Assessing the capacity of biochar to stabilize copper and lead in contaminated sediments using chemical and extraction methods

Because of its high adsorption capacity, biochar has been used to stabilize metals when remediating contaminated soils; to date, however, it has seldom been used to remediate contaminated sediment. A biochar was used as a stabilization agent to remediate Cu- and Pb-contaminated sediments, collected from three locations in or close to Beijing. The sediments were mixed with a palm sawdust gasified biochar at a range of weight ratios (2.5%, 5%, and 10%) and incubated for 10, 30, or 60?days. The performance of the different treatments and the heavy metal fractions in the sediments were assessed using four extraction methods, including diffusive gradients in thin films, the porewater concentration, a sequential extraction, and the toxicity characteristic leaching procedure. The results showed that biochar could enhance the stability of heavy metals in contaminated sediments. The degree of stability increased as both the dose of biochar and the incubation time increased. The sediment pH and the morphology of the metal crystals adsorbed onto the biochar changed as the contact time increased. Our results showed that adsorption, metal crystallization, and the pH were the main controls on the stabilization of metals in contaminated sediment by biochar.