ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Weiping Cai,Yujun Wang,Yu Feng,Peng Liu,Shuofei Dong,Bo Meng,Hua Gong,Fei Dang
Nanoparticulate mercury (Hg-NPs) are ubiquitous in nature. However, the lack of data on their concentration in soils impedes reliable risk assessments. This is due to the analytical difficulties resulting from low ambient Hg concentrations and background interferences of heterogeneous soil components. Here, coupled to single particle inductively coupled plasma-mass spectrometry (spICP-MS), a standardized protocol was developed for extraction and quantification of Hg-NPs in natural soils with a wide range of properties. High particle number-, particle mass-, and total mass-based recoveries were obtained for spiked HgS-NPs (74–120%). Indigenous Hg-NPs across soils were within 107–1011 NPs g–1, corresponding to 3–40% of total Hg on a mass basis. Metacinnabar was the primary Hg species in extracted samples from the Wanshan mercury mining site, as characterized by X-ray absorption spectroscopy and transmission electron microscopy. In agreement with the spICP-MS analysis, electron microscopy revealed comparable size distribution for nanoparticles larger than 27 nm. These indigenous Hg-NPs contributed to 5–65% of the measured methylmercury in soils. This work paves the way for experimental determinations of indigenous Hg-NPs in natural soils, which is critical to understand the biogeochemical cycling of mercury and thereby the methylation processes governing the public exposure to methylmercury.
研究领域:
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Hongqian Yin,Heng Yao,Wei Yuan,Che-Jen Lin,Xuewu Fu,Runsheng Yin,Bo Meng,Jun Luo,Xinbin Feng
Measuring the isotopic composition of Hg in natural waters is challenging due to the ultratrace level of aqueous Hg (ng L–1). At least 5 ng of Hg mass is required for Hg isotopic analysis. Given the low Hg concentration in natural waters, a large volume of water (>10 L) is typically needed. The conventional grab sampling method is time-consuming, laborious, and prone to contamination during transportation and preconcentration steps. In this study, a DGT (diffusive gradients in thin films) method based on aminopropyl and mercaptopropyl bi-functionalized SBA-15 nanoparticles was developed and extended to determine the concentration and isotopic composition of aqueous Hg for the first time. The results of laboratory analysis showed that Hg adsorption by DGT induces ∼ −0.2‰ mass-dependent fractionation (MDF) and little mass-independent fractionation (MIF). The magnitude of MDF exhibits a dependence on the diffusion-layer thickness of DGT. Since Hg-MDF can occur in a broad range of environmental processes, monitoring the δ202Hg of aqueous Hg using the DGT method should be performed with caution. Field results show consistent MIF signatures (Δ199Hg) between the DGT and conventional grab sampling method. The developed DGT method serves as a passive sampling method that effectively characterizes the MIF of Hg in waters to understand the biogeochemical cycle of Hg at contaminated sites.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
PubMed
高影响因子
TALANTA
·
2019
·
IF 4.916
Xiaoyu Jia,Junyi Zhao,Hongyun Ren,Jiani Wang,Zixiao Hong,Xian Zhang
Zwitterion-functionalized polymer microspheres (ZPMs) have been designed and used as the core adsorbent for the selective and rapid enrichment of mercury species in environmental waters by an on-line solid-phase extraction (SPE). Zwitterionic S-ZPMs and N-ZPMs having an anionic sulfonic group, but differing in cationic S + and N + moieties were prepared from Merrifield resin by treating with 1,2-ethanedithiol and imidazole , followed by modification with 1,3-propanesultone. Without any additional reagents, inorganic mercury (In-Hg), methylmercury (MeHg) and ethylmercury (EtHg) were quantitatively adsorbed on the home-made mini-column packed with ZPMs. Following extraction with 60 mM ammonium acetate and 0.15% L -cysteine ( L -Cys) solution within seconds, separation and speciation of mercury were successfully achieved by the HPLC–ICP-MS technique. Under the optimized experimental conditions, the enrichment factors (EFs) are up to 105 and 98 for inorganic and organic mercury only with 40 mL sample solution, respectively. The low detection limits of 0.78 ng L −1 , 0.63 ng L −1 , and 0.49 ng L −1 were reached for In-Hg, MeHg and EtHg, respectively, with the relative standard deviations (RSDs) below 4.1%. The feasibility and accuracy of the on-line SPE–HPLC–ICP-MS method were successfully applied for mercury speciation in surface water, seawater as well as certified reference material (CRM). The results here demonstrate a facile, sensitive and selective method for speciation of mercury at trace levels.
研究领域:
分析化学
·
环境科学
·
化工工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
·
2024
·
IF 9.7
Dingxi Zhang,Bowei Chu,Qingqing Yang,Xiaoyan Zhang,Yingying Fang,Guangliang Liu,Lina Liang,Yingying Guo,Yongguang Yin,Yong Cai,Guibin Jiang
Mercury (Hg), particularly organic mercury, poses a global concern due to its pronounced toxicity and bioaccumulation. Bioremediation of organic mercury in high-salt wastewater faces challenges due to the growth limitations imposed by elevated Cl − and Na + concentrations on microorganisms. In this study, an isolated marine bacterium Alteromonas macleodii KD01 was demonstrated to degrade methylmercury (MeHg) efficiently in seawater and then was applied to degrade organic mercury (MeHg, ethylmercury, and thimerosal) in simulated high-salt wastewater. Results showed that A. macleodii KD01 can rapidly degrade organic mercury (within 20 min) even at high concentrations (>10 ng/mL), volatilizing a portion of Hg from the wastewater. Further analysis revealed an increased transcription of organomercury lyase ( merB ) with rising organic mercury concentrations during the exposure process, suggesting the involvement of mer operon ( merA and merB ). These findings highlight A. macleodii KD01 as a promising candidate for addressing organic mercury pollution in high-salt wastewater.
研究领域:
环境微生物学
·
生物修复
·
海洋生物学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-15
·
IF 14.7
Li Hailong,Meng Fanyue,Zhu Penglin,Zu Hongxiao,Yang Zequn,Qu Wenqi,Yang Jianping
Highly efficient decontamination of elemental mercury (Hg 0 ) remains an enormous challenge for public health and ecosystem protection. The artificial conversion of Hg 0 into mercury chalcogenides could achieve Hg 0 detoxification and close the global mercury cycle. Herein, taking inspiration from the bio-detoxification of mercury, in which selenium preferentially converts mercury from sulfoproteins to HgSe, we propose a biomimetic approach to enhance the conversion of Hg 0 into mercury chalcogenides. In this proof-of-concept design, we use sulfur-rich polyphenylene sulfide (PPS) as the Hg 0 transporter. The relatively stable, sulfur-linked aromatic rings result in weak adsorption of Hg 0 on the PPS rather than the formation of metastable HgS. The weakly adsorbed mercury subsequently migrates to the adjacent selenium sites for permanent immobilization. The sulfur-selenium pair affords an unprecedented Hg 0 adsorption capacity and uptake rate of 1621.9 mg g −1 and 1005.6 μg g −1 min −1 , respectively, which are the highest recorded values among various benchmark materials. This work presents an intriguing concept for preparing Hg 0 adsorbents and could pave the way for the biomimetic remediation of diverse pollutants.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2014
·
IF 3.552
Guangzhu Li,Miao Liu,Zhuqing Zhang,Chao Geng,Zhongbo Wu,Xin Zhao
Surface sulfhydryl-functionalized magnetic mesoporous silica nanoparticles were prepared, aiming to extract trace alkylmercury from aqueous solution. The prepared nanoparticles were characterized by TEM, ED, EDX, DLS, FTIR, and SERS. Compare with that the non-sulfhydryl-functionalized Fe 3 O 4 @SiO 2 exhibited almost no affinity for CH 3 Hg + and CH 3 CH 2 Hg + ; the sulfhydryl-functionalized Fe 3 O 4 @SiO 2 exhibited high adsorption affinity for them, resulting from chelating interaction by surface sulfhydryl group, and the adsorption was not significantly impacted by pH within the range of 3.5–9.0 or coexisting metal ions. The monolayer adsorption on surface of Fe 3 O 4 @SiO 2 –RSH could reach equilibrium in 2 min. Moreover, the CH 3 Hg + and CH 3 CH 2 Hg + adsorbed on Fe 3 O 4 @SiO 2 –RSH could be quickly separated from the matrix in a magnetic field and desorbed easily by acetonitrile and l -cysteine aqueous solution or HCl solution, and the recoveries were more than 80%. Findings of the present work highlight the potential for using Fe 3 O 4 @SiO 2 –RSH magnetic nanoparticles as effective and reusable adsorbents for extraction of ultra trace alkylmercury from environmental water samples.
研究领域:
环境科学
·
纳米材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Yuping Xiang,Yingying Guo,Guangliang Liu,Yanwei Liu,Maoyong Song,Jianbo Shi,Ligang Hu,Yongguang Yin,Yong Cai,Guibin Jiang
Particle-bound mercury (HgP), ubiquitously present in aquatic environments, can be methylated into highly toxic methylmercury, but it remains challenging to assess its bioavailability. In this study, we developed anEscherichia coli-based whole-cell biosensor to probe the microbial uptake of inorganic Hg(II) and assess the bioavailability of HgP sorbed on natural and model particles. This biosensor can quantitatively distinguish the contribution of dissolved Hg(II) and HgP to intracellular Hg. Results showed that the microbial uptake of HgP was ubiquitous in the environment, as evidenced by the bioavailability of sorbed-Hg(II) onto particulate matter and model particles (Fe2O3, Fe3O4, Al2O3, and SiO2). In both oxic and anoxic environments, HgP was an important Hg(II) source for microbial uptake, with enhanced bioavailability under anoxic conditions. The composition of particles significantly affected the microbial uptake of HgP, with higher bioavailability being observed for Fe2O3 and lower for Al2O3 particles. The bioavailability of HgP varied also with the size of particles. In addition, coating with humic substances and model organic compound (cysteine) on Fe2O3 particles decreased the bioavailability of HgP. Overall, our findings highlight the role of HgP in Hg biogeochemical cycling and shed light on the enhanced Hg-methylation in settling particles and sediments in aquatic environments.
研究领域:
环境科学
·
微生物学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2021
·
IF 4.759
Dian-Bing Zhou,Ya-Bing Xiao,Fang Han,Ya-Ning Lv,Lei Ding,Wei Song,Yu-Xin Liu,Ping Zheng,Da Chen
A novel magnetic metal-organic frameworks (Fe 3 O 4 @UiO-66-SH) was successfully prepared by coating Fe 3 O 4 nanospheres with sulfur-functionalized UiO-66. The Fe 3 O 4 @UiO-66-SH possesses both the magnetic properties of Fe 3 O 4 and the diverse properties of metal-organic framework (MOF) in one material, which has the superiority of high surface area, easy-operation and strong adsorb ability with mercury, is used for the magnetic solid-phase extraction of methylmercury (MeHg + ) and inorganic mercury (Hg 2+ ) in water and fish samples. The analyzes were conducted by high performance liquid chromatography-inductively coupled plasma mass spectrometry (HPLC-ICP-MS). The different pretreatment conditions influencing the extraction recoveries of Hg 2+ and MeHg + , including adsorbent amount, pH, extraction time, elution solvent, elution volume, desorption time, co-existing ions and dissolved organic materials were investigated. Under the optimized conditions, the limits of detection (LODs) of Hg 2+ and MeHg + for water samples were 1.4 and 2.6 ng L −1 , and the limits of quantification (LOQs) of Hg 2+ and MeHg + for water samples were 4.7 and 8.7 ng L −1 . The enrichment factors (EFs) were 45.7 and 47.6 fold for Hg 2+ and MeHg + , respectively. The accuracy of the proposed method was demonstrated by analyzing the certified reference material of fish tissue (GBW10029) and by determining the analyte content in spiked water and fish samples. The determined values were in good agreement with the certified values and the recoveries for the spiked samples were in the range of 84.5–96.8%.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
高影响因子
Surfaces and Interfaces
·
2018
·
IF 0
Jinrong Lu,Xiaonan Wu,Yao Li,Wenquan Cui,Yinghua Liang
The electron-donating group dithiocarbamate functionalized silica gel (SG-PDC) was prepared and used for adsorption of metal ions from aqueous solution. The modified silica gel was characterized by fourier transform infrared spectroscopy (FT-IR), elemental analysis (EA) and scanning electron microscopy (SEM). It showed excellent adsorption selectivity for Hg(II) ions over other metal ions, such as Cu(II), Cd(II), Pb(II). Kinetics and equilibrium isotherms of Hg (II) sorption were determined in batch equilibrium experiments. The adsorption capacity for Hg (II) of SG-PDC was more than five times as much as that of unmodified silica gel. X-ray photoelectron spectroscopy (XPS) was applied to study the adsorption mechanism and it confirmed that the improvement in mercury adsorption was related to the ligand groups containing S and N atoms anchored on the surface of silica gel. The adsorbent had high reusability after several adsorption–desorption cycles. This study provided a feasible strategy to develop the effective sorbent for Hg (II) ions by covalently modification of silica gel with ligand containing multiple coordination sites.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
·
2025
·
IF 6.1
Hangyu Lin,Yanlin Wei,Junjie Huang,Qun Lu,Song Zhu,Jianguang Qin,Shengqi Su,Tao He
Mercury poses significant hazards to aquatic organisms, causing neurotoxicity, and metabolic disorders. Research on the dynamic distribution of mercury within zooplankton is limited, and the metabolic mechanisms of mercury in zooplankton remain unclear. In this study, we employed a mercury-specific fluorescent probe (aggregation-induced emission luminogen, AIEgen) to visualize the in vivo distribution of Hg 2 + and MeHg in brine shrimp. Both Hg 2+ and MeHg accumulated predominantly in the head, ocellus, midgut, and midgut–hindgut transition, with Hg 2+ further affecting the hindgut and anal opening. Transcriptomics and metabolomics analyses revealed that Hg 2+ exposure in the midgut likely induced the efflux activity of ABC transporters. The linoleic acid metabolism, α-linolenic acid metabolism, tryptophan metabolism, and retinol metabolism pathways were potentially associated with MeHg accumulation in the head and ocellus. Additionally, the cytochrome P450 pathway participated in detoxification. Enzyme assays and multi-omics data further demonstrated that both Hg 2+ and MeHg elicited oxidative stress and impaired growth, development, and energy metabolism in brine shrimp. Integrated omics analysis revealed that glutathione metabolism is highly associated with Hg 2+ , while glycerophospholipid metabolism is highly associated with MeHg. Our study revealed the toxicity effects of mercury in zooplankton brine shrimp and promoted the understanding of the underlying mechanism and coping strategies for mercury toxicity in the zooplankton of the aquatic food chain.
研究领域:
生态毒理学
·
海洋生物学
·
环境科学
·
分子生物学
·
生物信息学
·
毒理学
·
浮游动物研究
✓ 已验证
DOI
PubMed
高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Yuping Xiang,Yueqian Chen,Yingying Guo,Yanwei Liu,Guangliang Liu,Yongguang Yin,Dingyong Wang,Yong Cai,Guibin Jiang
How organic ligands regulate microbial Hg(II) bioavailability remains a critical knowledge gap in elucidating methylmercury production and subsequent bioaccumulation in biota. Six model ligands with different functional groups (ethylenediaminetetraacetate [EDTA], citrate [CTA], cysteine [CYS], glutathione [GSH], 2, 3-dimercapto-1-propanesulfonate [DMPS], and 3-mercapto-1-propanesulfonate [MPS]) were applied to probe their impacts on Hg(II) bioavailability, by direct measurement of active cellular Hg(II) and cell physiology using a Hg(II)-specific ( Escherichia coli PRL) and a constitutive biosensor ( E. coli PJL), respectively. Hg(II) uptake was significantly inhibited by EDTA, CTA, DMPS, and MPS, whereas enhanced by CYS and GSH. These findings indicate co-occurred uptake mechanism other than the widely accepted membrane-ligand exchange model, since bioavailability did not inversely correlate with Hg-binding strength (CTA < EDTA < GSH < CYS < DMPS). Furthermore, ligand-induced bacterial physiological changes (e.g., thiolate inhibition vs. carboxylate neutrality) were not the primary driver of bioavailability variations. Based on Hg(II) speciation analysis and thermodynamic modelling, it was implied that sulfate reduction and CYS degradation generated sulfide corona near bacterial cells, promoting the formation of Hg sulfide nanoparticles (HgS NP ) or Hg-S clusters during Hg(II) uptake. Enhanced bioavailability of Hg(II)-CYS/GSH likely arose from passive diffusion and intracellular dissolution of these HgS species. Ambient oxygen levels further modulate Hg(II) bioavailability, with enhanced Hg(II)-CYS uptake observed under anoxic conditions, likely due to oxygen-dependent transporters expression and bacterial metabolisms. Overall, these findings highlight ligand-specific mechanisms governing Hg(II) bioavailability, emphasizing the interactions of Hg-binding strength, cell physiology, and sulfide-driven speciation in Hg biogeochemical cycling.
研究领域:
环境微生物学
·
生物地球化学
·
环境化学
·
微生物生理学
·
毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Hui Wang,Wangsheng Yu,Xu Peng,Zewen Chen,Shengji Wu,Qinqin Yu,Wei Yang,Jie Zhou
In the present work, highly efficient catalytic adsorbents for Hg 0 removal in both oxygen-rich and deficient atmosphere are developed based on an “adaption” strategy. Firstly, a series of simplified SiO 2 -based catalytic adsorbents are prepared as model catalysts to gain a deeper insight into the mechanism of the catalytic Hg 0 removal process. It is found that for the effective Hg 0 removal, the catalytic adsorbent should possess an “assembling” structure involving both Hg 0 and oxygen activation sites. An “adaption” strategy is thus implemented for the devise of the catalytic adsorbent, including the functional adaption of different active sites for the reactants and the synergistic function of different active sites. Accordingly, high-efficiency catalytic adsorbent with strong redox property is developed for oxygen-rich atmosphere, while the catalytic adsorbent with high oxygen storage/release property is developed for oxygen-deficient conditions. Moreover, regeneration investigation indicates that the activities of spent catalytic adsorbents are almost fully recovered through the temperature programmed decomposition and desorption (TPDD) process. It is believed that the present “adaption” strategy for catalyst design has guiding significance for the rational and controllable construction of catalysts for other catalytic processes.
研究领域:
环境催化
·
大气污染控制
·
材料化学
·
表面科学
·
化学工程
·
环境功能材料
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）