CHEMOSPHERE
·
2022
·
IF 8.943
Kai-Qiang He,Xiao-Ru Zhang,Yuan-Peng Li,Xue-Lei Duan,Yan Li,Yang-Hong Jiang,Xiao-Dong Yuan,Ke-Gang Zhang,Chun-Gang Yuan
Along with the environmental protection policies becoming strict in China, the air pollution control devices (especially selective catalytic reduction (SCR)) are widely equipped in coal-fired power plants. The installation and run of these devices will inevitably affect mercury (Hg) species distribution in coal fired by-products such like fly ash (FA) and gypsum. In this work, a new on-line coupling system based on atomic fluorescence spectrometry (AFS) with a home-made chromatographic workstation was successfully developed to identify Hg species through thermal programmed desorption (TPD). The influences of matrix, furnace temperature, and carrier gas flow on analytical performance were investigated and the parameters were optimized. The FA and gypsum samples from coal-fired power plants equipped with SCR were collected and the mercury species were analyzed by the developed coupling system. HgCl 2 and HgO were the main species in FA, while Hg 2 Cl 2 and HgO were the main species in gypsum. All of Hg species in the studied FA and gypsum samples were released below 400 °C. A sequential extraction procedure was applied to further verify the operational Hg species including mobile and non-mobile fractions in FA and gypsum samples. This study demonstrated that AFS coupled with TPD procedure was an effective method to analyze Hg species in coal combustion by-products from power plants.
研究领域:
环境科学
·
能源与燃料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2025
·
IF 8
Siqi Wu,Chen Yang,Haochen Xu,Yiwei Zhu,FengFu Fu,Yue Lin
The contamination of micro-plastics (MPs)/nano-plastics (NPs) in environment poses a global concern, necessitating a scientific evaluation of their potential risks to ecosystems and organisms. We herein investigated the adsorption kinetics of different mercury species including inorganic mercury (Hg 2+ ), methylmercury (MeHg) and ethylmercury (EtHg) on three different MPs, such as polyethylene MPs (PE MPs), polypropylene MPs (PP MPs) and polystyrene MPs (PS MPs) in micro-polluted water in detail, and further evaluated the individual and combined cytotoxicity of polystyrene NPs (PS NPs)/polypropylene NPs (PP NPs) and different mercury species. The results indicated that EtHg undergoes demethylation partly to form Hg 2+ during the adsorption process on PP MPs, and the adsorption kinetics of Hg 2+ , MeHg and EtHg on three MPs fitted with pseudo-first-order (PFO) model in initial stage and simultaneously fitted with pseudo-second-order (PSO) model during whole adsorption process. This suggested that adsorption of mercury species on three MPs we driven mainly by physical process in initial stage and by chemical process during whole absorption process. In natural micro-polluted water, the equilibrium adsorption capacities (Q e ) of Hg 2+ on three MPs (156.3–270.3 ng/g) are much higher than that of MeHg (5.562–78.13 ng/g) and EtHg (7.831–70.42 ng/g). Cytotoxicity experiments revealed that PP NPs and PS NPs themselves have little cytotoxicity, but the presence of them can enhance the cytotoxicity of mercury species, showing NPs size-depended and mercury species-depended synergistic toxic effect. The findings of this study provided valuable insights for scientifically evaluating the potential risk of MPs/NPs to ecosystems and organisms.
研究领域:
环境科学
·
毒理学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2014
·
IF 5.9
Ling Chen,Jinhua Li,Lingxin Chen
The speciation analysis of heavy metal pollutants is very important because different species induce different toxicological effects. Nanomaterial-assisted optical sensors have achieved rapid developments, displaying wide applications to heavy metal ions but few to metal speciation analysis. In this work, a novel colorimetric nanosensor strategy for mercury speciation was proposed for the first time, based on the analyte-induced aggregation of gold nanoparticles (Au NPs) with the assistance of a thiol-containing ligand of diethyldithiocarbamate (DDTC). Upon the addition of mercury species, because Hg-DDTC was more stable than Cu-DDTC, a place-displacement between Hg species and Cu2+ would occur, and thereby the functionalized Au NPs would aggregate, resulting in a color change. Moreover, by virtue of the masking effect of ethylenediaminetetraacetic acid (EDTA), the nanosensor could readily discriminate organic mercury and inorganic mercury (Hg2+), and it is thus anticipated to shed some light on the colorimetric sensing of organic mercury. So, a direct, simple colorimetric assay for selective determination of Hg species was obtained, presenting high detectability, such as up to 10 nM for Hg2+ and 15 nM for methylmercury. Meanwhile, the strategy offered excellent selectivity toward mercury species against other metal ions. The simple, rapid, and sensitive label-free colorimetric sensor for the determination of Hg species provided an attractive alternative to conventional methods, which usually involve sophisticated instruments, complicated processes, and long periods of time. More importantly, by using mercury as a model, an excellent nanomaterial-based optical sensing platform can be developed for speciation analysis of trace heavy metals, which can lead to nanomaterials stability change through smart functionalization and reasonable interactions.
研究领域:
分析化学
·
环境科学
·
纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2025
·
IF 4
Jiahui Shi,Zhenhua Wang,Jingbo Chao,Ligang Hu,Bing Li,Caifeng Dai
Covalent organic frameworks (COFs) with low chemical or thermal stability may lead to destruction of their molecular structure when used under harsh conditions and environments, thereby limiting their use in practical processes. A magnetic COFs nano-adsorbent (Fe 3 O 4 @COF-TF) was prepared by coating thianthrene-based COFs with high chemical and thermal stability onto Fe 3 O 4 nanoparticles by a simple solvothermal method without post-modification to introduce the target functional groups. Based on the above nano-adsorbent, a simple and practical magnetic solid-phase extraction–high-performance liquid chromatography–inductively coupled plasma mass spectrometry (MSPE-HPLC-ICP-MS) method was developed for the enrichment and determination of trace mercury species, including Hg 2+ , methylmercury (MeHg), and ethylmercury (EtHg). The experimental results showed that Fe 3 O 4 @COF-TF could still recover mercury species quantitatively after acid and alkali soaking treatment or 35 consecutive adsorption-desorption cycles. This indicates Fe 3 O 4 @COF-TF had excellent durability, extraction stability and reusability. Key parameters affecting the enrichment of mercury species, including solution pH, eluent composition and volume, adsorption and desorption time and dissolved organic matter, were systematically optimized. Under optimized conditions, the limits of detections (LODs) for Hg 2+ , MeHg and EtHg were 0.50, 0.19 and 0.67 ng L −1 based on 300 mL of sample, with enrichment factors (EFs) of 338, 356 and 329, respectively. The accuracy and reproducibility of the method were validated through spiked tests and determination of certified reference materials. The developed method with the advantages of simplicity, high anti-interference capability, high enrichment factor and high sensitivity was successfully applied to the enrichment and determination of trace mercury in groundwater, surface water, seawater, and other complex matrices.
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
JOURNAL OF CHROMATOGRAPHY A
·
2022
·
IF 4.601
Haokun Zhang,Youfang Huang,Xiaochong Song,Jinghe Peng,Yiqi Xu,Yu Zhang,Xiaojia Huang
Efficient extraction is a vital step in mercury speciation. In this context, using 4-vinylbenzeneboronic acid and 9-vinylanthracene as functional monomers, a new magnetic adsorbent was fabricated according to one-pot hydrothermal approach. Various characterization results prove the as-prepared adsorbent presented abundant functional groups and saturation magnetism. Combining with magnetic solid phase extraction (MSPE), the adsorbent exhibited satisfactory entrapment performance towards different mercury species which had been pre-coordinated with dithizone to form metal-organic coordination. A series of parameters influencing the extraction performance were inspected in detail. Under the most beneficial conditions, sensitive and reliable approach to quantify trace methylmercury, ethylmercury, phenylmercury and inorganic mercury in aqueous samples was developed by the combination of HPLC/DAD. Limits of detection and precision located in the ranges of 0.012–0.074 µg/L and 2.5–9.8%, respectively. Recoveries with low, medium and high fortified contents in actual waters varied from 79.8 to 119%. Confirmatory experiments were performed to evidence the accuracy and reliability of established approach. In addition, a possible mechanism was suggested based on the chemical nature of analytes, extraction conditions and characterization results.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yanyan Gong,Jie Yin,Tong Zhang,Weizhao Yin,Luyao Sun,Qiru Liang,Qilin Wang
Mercury speciation in groundwater affects its removal effectiveness and methylation potential. Yet, most studies focus on the removal of inorganic dissolved Hg(II) and few studies explored the mercury methylation before and after the treatment. This study comprehensively explored the removal performance of three model mercury species, namely, dissolved inorganic divalent Hg (Hg(II), including free Hg 2+ and Hg 2+ complexes with Cl − and OH − ), Hg 2+ bound to dissolved organic matter (Hg-DOM), and HgS nanoparticles by FeS nanoparticles and further investigated the resultant impacts on the microbial methylation of Hg. Among three different stabilizers (starch, carboxymethyl cellulose (CMC), carboxymethyl starch (CMS)), CMC stabilized FeS nanoparticles (CMC-FeS) demonstrated best physical stability and highest mercury uptake. The CMC-FeS nanoparticles efficiently immobilized the three mercury species within 20 h. The sorption isotherm data of Hg(II) and Hg-DOM were well fitted by the dual-mode isotherm model and the maximum sorption capacities were 3358.28 and 2396.38 mg/g, respectively. Hg(II) and Hg-DOM were predominantly removed via ion exchange, chemical precipitation, and surface complexation whereas HgS was mainly immobilized through heteroaggregation. The simple treatment greatly reduced the bioavailable Hg species, thereby diminishing the net MeHg production by 70.2 %, 32.7 %, and 11.3 %, respectively. This study provides compelling evidence that FeS nanoparticles efficiently removed various mercury species in groundwater and remarkably inhibited the microbial methylation of mercury.
研究领域:
环境科学
·
微生物学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Xiaochong Song,Jiangyi Wu,Jinling Pang,Yuanfei Wu,Xiaojia Huang
In this study, a novel sorbent based on task specific monolith doped with Fe 3 O 4 was in situ fabricated in capillary and acted as the extraction medium of magnetic field-reinforced in-tube solid phase microextraction (MFR/IT-SPME) to trap and preconcentrate mercury species which were coordinated with dithizone to form chelates. Various characterization technologies evidenced that the obtained monolithic adsorbent presented porous and super paramagnetic properties, and possessed abundant functional groups. Results evidenced that the implementation of magnetic field during extraction stages enhanced the extraction efficiency of studied Hg chelates from 48.5% to 75.3% to 69.9–94.4%. Under the optimized extraction parameters, the introduced MFR/IT-SPME was online coupled to HPLC/DAD to quantify mercury species at ultra-trace levels in various water samples. Limits of detection varied from 0.0067 μg/L to 0.016 μg/L, and the RSDs for precision were below 7.5%. Additionally, related extraction mechanism was deduced and revealed multiple forces co-contributed to the enrichment. The reliability and accuracy of suggested online approach for speciation analysis of mercury was well proved by confirmatory experiments.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Ying Wang,Guangliang Liu,Yingying Fang,Peng Liu,Yanwei Liu,Yingying Guo,Jianbo Shi,Ligang Hu,Yong Cai,Yongguang Yin,Guibin Jiang
Liquid elemental mercury droplet (Hg(0) l ) is an important species in heavy Hg-contaminated environments. The oxidation processes of Hg(0) l and its related mechanisms are still poorly understood. Herein, for the first time, it was verified that mercurous species [Hg(I)] was an important species in natural water contaminated by Hg(0) l as well as in the simulated dark oxidation of Hg(0) l . The formation and further transformation of Hg(I) controlled the overall oxidation process of Hg(0) l and were affected by different environmental factors. Through kinetic modeling using ACUCHEM program, oxidation of Hg(0) to Hg(I) (Hg(0) → Hg(I)) was determined to be the rate-limiting step in Hg(0) l oxidation because its k value ((8.7 ± 0.21) × 10 −11 s −1 ) is seven orders of magnitude lower than that of Hg(I) oxidation (Hg(I) → Hg(II), (4.7 ± 0.15) × 10 −4 s −1 ). Ligands like OH − , Cl − , and natural organic matter enhanced the formation of Hg(I) via promoting the constants of comproportionation (up to (9.5 ± 0.78) × 10 −4 s −1 ). These findings highlight the importance of Hg(I) in Hg(0) l oxidation process by controlling the transformation kinetics of Hg species, facilitating an improved understanding of the environmental redox cycles of Hg.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROPHORESIS
·
2018
·Vol. 39
·期 14
·1763-1770
·
IF 2.569
Jinhua Li,Junying Liu,Wenhui Lu,Fangfang Gao,Liyan Wang,Jiping Ma,Huitao Liu,Chunyang Liao,Lingxin Chen
A pretreatment method of dispersive solid-phase extraction (DSPE) along with back-extraction followed by CE-UV detector was developed for the determination of mercury species in water samples. Sulfhydryl-functionalized SiO 2 microspheres (SiO 2 −SH) were synthesized and used as DSPE adsorbents for selective extraction and enrichment of three organic mercury species namely ethylmercury (EtHg), methylmercury (MeHg), and phenylmercury (PhHg), along with L-cysteine (L-cys) containing hydrochloric acid as back-extraction solvent. Several main extraction parameters were systematically investigated including sample pH, amount of adsorbent, extraction and back-extraction time, volume of eluent, and concentration of hydrochloric acid. Under optimal conditions, good linearity was achieved with correlation coefficients over 0.9990, in the range of 4−200 μg/L for EtHg, and 2−200 μg/L for MeHg and PhHg. The LODs were obtained of 1.07, 0.34, and 0.24 μg/L for EtHg, MeHg, and PhHg, respectively, as well as the LOQs were 3.57, 1.13, and 0.79 μg/L, respectively, with enrichment factors ranging from 109 to 184. Recoveries were attained with tap and lake water samples in a range of 62.3−107.2%, with relative standard deviations of 3.5–10.1%. The results proved that the method of SiO 2 −SH based DSPE coupled with CE-UV was a simple, rapid, cost-effective, and eco-friendly alternative for the determination of mercury species in water samples.
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 Methods
·
2024
·
IF 2.7
Shengji Wu,Guiyuan Hu,Yutao Shen,Rui Tang,Fan Yang,Lei Che,Wei Yang
Determination of mercury species over solid waste from natural gas processing plants is a prerequisite for solid waste decontamination and mercury recycling. The temperature-programmed decomposition and desorption method (TPDD) is a promising technique to determine the mercury species over solid waste. Mercury species over solid wastes with complex components and similar desorption temperature, however, cannot always be determined using only the TPDD method. In the present study, the EPA 3200 method was applied to optimize the TPDD process for speciation of the mercury compound over solid wastes collected from a natural gas processing plant, including four spent adsorbents and three sludges. The mercury species with similar desorption temperatures over solid wastes were completely separated by EPA 3200 method optimized TPDD process. The mercury species over spent adsorbents and sludges could be determined based on the fingerprints of the mercury compounds. The mercury compounds over spent adsorbent were specified to be Hg0 and/or M-Hg amalgam, HgS(Black) and HgO(Red), of which HgS(Black) was the primary mercury compound. However, the mercury species over sludge were analyzed to be Hg0 and/or M-Hg amalgam, HgCl2(minor), HgS(Black), HgO(Yellow) and HgS(Red). The mercury recovery rates of solid wastes ranged from 73% to 120%. With the above results, it was considered that the EPA 3200 method optimized TPDD process was a promising method to specify and semi-quantify the mercury compounds in solid waste.
研究领域:
环境科学
·
分析化学
·
废物管理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2017
·
IF 3.981
Heyong Cheng,Xiaopan Chen,Lihuan Shen,Yuanchao Wang,Zigang Xu,Jinhua Liu
Most of analytical community is focused on reversed phase high performance liquid chromatography (RP-HPLC) for mercury speciation by employing mobile phases comprising of high salts and moderate amounts of organic solvents. This study aims at rapid mercury speciation analysis by ion-pairing RP-HPLC with inductively coupled plasma mass spectrometry (ICP-MS) detection only using low salts for the sake of green analytical chemistry. Two ion-pairing HPLC methods were developed on individual usage of positively and negatively charged ion-pairing reagents (tetrabutylammonium hydroxide –TBAH and sodium dodecylbenzene sulfonate –SDBS), where sodium 3-mercapto-1-propysulfonate (MPS) and l -cysteine (Cys) were individually added in mobile phases to transform mercury species into negative and positive Hg-complexes for good resolution. Addition of phenylalanine was also utilized for rapid baseline separation in combination of short C 18 guard columns. Optimum mobile phases of 2.0 mM SDBS + 2.0 mM Cys + 1.0 mM Phe (pH 3.0) and 4.0 mM TBAH + 2.0 mM MPS + 2.0 mM Phe (pH 6.0) both achieved baseline separation of inorganic mercury (Hg 2+ ), methylmercury (MeHg), ethylmercury (EtHg) and phenylmercury (PhHg) on two consecutive 12.5-mm C 18 columns. The former mobile phase was selected for mercury speciation in freshwater fish because of short separation time (3.0 min). Detection limits of 0.015 for Hg 2+ , 0.014 for MeHg, 0.028 for EtHg and 0.042 μg L −1 for PhHg were obtained along with satisfactory precisions of peak height and area (1.0-2.8% for 5.0 μg L −1 Hg-mixture standard). Good accordance of determined values of MeHg and total mercury in certified reference materials of fish tissue (GBW 10029) and tuna fish (BCR-463) with certified values as well as good recoveries (91–106%) proved good accuracy of the proposed method. An example application to freshwater fish indicated its potential in routine analysis, where MeHg was presented at 3.7–20.3 μg kg −1 as the dominate species.
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
JOURNAL OF CHROMATOGRAPHY A
·
2024
·
IF 3.8
Heping Jiao,Ruixiang Bi,Fangli Li,Jingbo Chao,Guimin Zhang,Lihai Zhai,Ligang Hu,Zhenhua Wang,Caifeng Dai,Bing Li
The complex and cumbersome preparation of magnetic covalent organic frameworks (COFs) nanocomposites on a small scale limits their application. Herein, a rapid and easy route was employed for the preparation of magnetic thiourea-based COFs nanocomposites. COFs were coated on Fe 3 O 4 nanoparticles at room temperature without a catalyst within approximately 30 min. This method is suitable for the large-scale preparation of magnetic adsorbent. Using the as-prepared magnetic adsorbent (Fe 3 O 4 @COF-TpTU), we developed a simple, efficient, and sensitive magnetic solid-phase extraction-high performance liquid chromatography-inductively coupled plasma-mass spectrometry (MSPE-HPLC-ICP-MS) for the enrichment and determination of mercury species, including Hg 2+ , methylmercury (MeHg), and ethylmercury (EtHg). The effects of the experimental parameters on the extraction efficiency, including solution pH, adsorption and desorption time, composition and volume of the elution solvent, salinity, coexisting ions, and dissolved organic matter, were comprehensively investigated. Under optimised conditions, the limits of detection in the developed method were 0.56, 0.34, and 0.47 ng L −1 with enrichment factors of 190, 195, and 180-fold for Hg 2+ , MeHg, and EtHg, respectively. The satisfactory spiked recoveries (97.0–103%) in real water samples and high consistency between the certified and determined values in a certified reference material demonstrate the high accuracy and reproducibility of the developed method. The as-proposed method with simple operation, high sensitivity, and excellent anti-matrix interference performance was successfully applied to the enrichment and determination of trace levels of mercury species in the natural samples with complicated matrices, such as underground water, surface water, seawater and biological samples.
研究领域:
分析化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）