Journal of Water Process Engineering
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2022
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IF 7.34
Xu Chai,Huaqi Dong,Zenggao Zhang,Zhaoyang Qi,Jie Chen,Zhixian Huang,Changshen Ye,Ting Qiu
Due to natural and production activities, mercury contamination has become one of the major environmental problems in the world. Adsorption is one of the important means to solve this problem. However, most of the commercially available adsorbents exhibit relatively low adsorption capacity and slow kinetics. Therefore, a novel 4,6-diamino-2-mercaptopyrimidine-functionalised Zr-based metal-organic framework (UiO-66-DMP) was synthesised in this study. The UiO-66-DMP was characterised through X-ray diffraction, scanning electron microscopy, energy dispersive spectrometry , X-ray photoelectron spectroscopy, Fourier-transform infrared spectrometry, and thermogravimetric analysis . The potential of the UiO-66-DMP as a superior adsorbent for Hg(II) removal and the corresponding mechanisms were evaluated through batch experiments under different conditions and density functional theory calculations. Benefitting from its high specific surface area and multiple adsorption sites, the maximum Hg(II) adsorption capacity achieved in this study was 822.00 mg·g-1, which is the highest Hg(II) adsorption capacity reported to date. In addition, under the interference of Ca(II), Cd(II), Co(II), Mg(II), Mn(II), Ni(II), Cr(III), Cu(II), Zn(II) and other coexisting ions, the UiO-66-DMP could still maintain the high selective adsorption capacity for Hg(II). According to the characterization analysis and DFT calculation results, the adsorption of Hg(II) onto the UiO-66-DMP was dependent on electrostatic and covalent interactions between metal ions and abundant functional groups on the UiO-66-DMP surface.
研究领域:
环境科学
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材料科学
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化学工程
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高影响因子
MICROCHIMICA ACTA
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2019
·Vol. 186
·期 5
·1-6
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IF 5.479
Ma Haiyan,Xue Ning,Wu Shujie,Li Zongbing,Miao Xiangmin
The authors describe a method for detection of Hg 2+ by using positively charged gold nanoparticles ((+)AuNPs) as a quencher of the fluorescence of DNA-capped silver nanoclusters (DNA-AgNCs) which are negatively charged. In the presence of Hg 2+ , a DNA duplex is formed through T-Hg 2+ -T coordination chemistry. The duplex can be digested by exonuclease III to form smaller DNA fragments. This leads to the release of the AgNCs and the recovery of fluorescence, best measured at excitation/emission wavelengths of 460/530 nm. The (+)AuNPs and Hg 2+ are also released and can be reused for target recycling signal amplification. Based on these findings, a method is worked out for the determination of Hg 2+ that works in the 5.0 pM to 10 nM concentration range and has a detection limit as low as 2.3 pM. It is highly selective because of the highly specific formation of T-Hg 2+ -T bonds.
By using ultrastable and positively charged gold nanoparticles as fluorescence quenchers and exonuclease assisted signal amplification, a method is developed for the sensitive and selective detection of Hg 2+ in water samples.
研究领域:
分析化学
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环境科学
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PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Junyang Wang,Caiyi Du,Peitong Yu,Qian Zhang,Hongxia Li,Chunyan Sun
A label-free and enzyme-free signal-on biosensor for Hg(II) ions was constructed based on T-Hg(II)-T nanoladders and fluorescent DNA-templated silver nanoclusters/graphene oxide nanocomposites (DNA-AgNCs/GO). The T-rich sequences (P1 and P2) were used to capture Hg(II) and form the T-Hg(II)-T nanoladders. C 6 G 5 C 6 was extended at the 5′ end of P1, used as a template for synthesizing fluorescent DNA-AgNCs. In the presence of mercury ions , the T-Hg(II)-T nanoladders significantly enhanced the emission of AgNCs. GO can attract free P1-C 6 G 5 C 6 and P2 that were not involved in the formation of T-Hg(II)-T nanoladders, thus employed as the energy acceptor to quench the background fluorescence of AgNCs. The fluorescence enhancement induced by mercury ions can be used for quantitative detection of Hg(II) over the range 0.1–30 nM with a detection limit as low as 7.35 pM. This method was used to detect Hg(II) in the spiked samples of Songhua River water and grass carp, with the recoveries of 97.61%− 103.79% and 96.52%− 105.58% respectively, consistent with the results from atomic fluorescence spectrometry. Obviously, in this assay, enzyme-free signal amplification and signal identification are integrated in the ingenious design of nucleic acid sequences, thus achieving the label-free fluorescence detection of mercury ions.
研究领域:
生物化学
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环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2019
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IF 8.456
Lei Wang,Yu Wang,Wenxuan Li,Wenjing Zhi,Yuanyuan Liu,Liang Ni,Yun Wang
Going beyond organic solvent as the solubilizer for small-molecular organic probes motivates exploration of water-soluble polymeric sensors. In this respect, dye-derived thermal-responsive polymeric sensors are an attractive direction, but for its practical application, it is limited by sensor recycling because only irreversible change in the structure of the recognition unit for many sensors can trigger the appearance of the detection signal. Here, we established the oligonucleotide-derived thermal-responsive polymeric sensor, TBC-P1, which overcame this fundamental limitation. The TBC-P1 sensor was based on reversible binding between oligonucleotides and Hg2+ ions, and easy sensor separation via tuning temperature, achieving the Hg2+ detection in a cost-effective and green manner. The TBC-P1 sensor displayed specific and rapid sensing properties toward Hg2+ ions in pure aqueous media via turn-off fluorescence emission, with a limit of detection as low as 0.65 nM (much lower than the presently reported dye-derived polymeric sensors). This high detection sensitivity was further enhanced (with LOD = 0.17 nM) via warming to yield spherical micelles, in which the oligonucleotide-containing thermoresponsive PNIPAM block forming a hydrophobic core amplified the fluorescence signals. Treating the Hg2+-trapped micelles with cysteine (Cys) led to competition-induced release of these combined Hg2+ ions and then thermally precipitating and recycling polymeric sensor TBC-P1. This oligonucleotide-derived thermalresponsive polymeric sensor will open a universal avenue for sensor recycling, which will achieve the goal of reducing cost and improving detection sensitivity of sensors.
研究领域:
材料科学
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分析化学
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环境科学
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纳米技术
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Ming Li,Panpan Zhang,Xuemeng Zhang,Qian Chen,Qianyong Cao,Yuling Zhang,Huining Xiao
Mercury pollution in aqueous solutions is a severe problem in environmental protection and the contaminated water may cause serious risks to human health. Based on the constant development of adsorptive materials, adsorption technique is widely applied as an efficient and convenient approach to eliminate mercury species from waters. In this work, we report a one-pot procedure to prepare a bis-Schiff base cellulosic adsorbent to integrate the advantages of large adsorptive capacity and excellent fluorescent recognition towards mercury ions. The adsorption experiments demonstrate that sulfydryl-contained cellulosic nanocrystals exhibit specific affinity with mercury species and the adsorption capacity reaches as high as 624.8 mg/g at room temperature. Besides, the introduction of rhodamine moiety endows the material a 19 times enhancement of selective “off-on” fluorescent sensing while exposed to mercury. Additionally, the bifunctional adsorbent material shows high sensitivity towards mercury ions in aqueous solution with detection limits of as low as 8.29 × 10 −8 M for fluorescence and 5.9 × 10 −9 M for UV–vis spectrum, respectively. The fitting results of the adsorption models indicate a monolayer adsorption during the uptake of mercury ions and the removal process follows the pseudo-second order kinetics. Moreover, density functional theory studies are employed to further understand the adsorptive and responsive mechanisms.
研究领域:
环境科学
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材料科学
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分析化学
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PubMed
高影响因子
WATER RESEARCH
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2025
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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
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生物地球化学
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环境化学
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微生物生理学
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毒理学
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 32
·14724-14738
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IF 3.591
Lin Qian,Zheng Zeng,Shuyuan Zhang,Kai Xia,Yongfu Guo
In the present work, a poly-o-vanillin-functionalized magnetic nanoparticle of PoVan/CoFe2O4@mSiO2 with core–shell structure was synthesized through a facile, green and low cost method. The rapid removal of Hg(II) by the prepared nanocomposites was researched by batch adsorption experiments and the adsorption conditions were optimized with response surface methodology (RSM). The optimization of RSM shows that the as-prepared PoVan/CoFe2O4@mSiO2 magnetic nanomaterial has a maximal adsorption capability of 263.6 mg g−1 toward Hg(II) ions. The removal process of Hg(II) ions acts in accordance with Langmuir and pseudo-second-order kinetic models. The Dubinin-Radushkevich calculation indicates that the removal process is spontaneous and exothermic. In addition, the adsorption of Hg(II) ions onto PoVan/CoFe2O4@mSiO2 is mainly completed through forming a stable complex by electrostatic attraction and chelation. The adsorption efficiency of the regenerated adsorbent is still high after five cycles. The used adsorbent of PoVan/CoFe2O4@mSiO2 has good magnetic property and can easily be separated from aqueous solution. The results indicate that the magnetic nanomaterial PoVan/CoFe2O4@mSiO2 could be a promising adsorbent to remediate mercury pollution from wastewater.
研究领域:
环境科学
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材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yifan Li,Tianliang Hu,Run Chen,Rong Xiang,Qiang Wang,Yongfei Zeng,Chiyang He
A novel thiol-functionalized covalent organic framework (COF-S-SH) was prepared as an adsorbent for the simultaneous removal of BTEX (benzene, toluene, ethyl benzene and xylenes) and Hg(II) ion from water. The COF-S-SH was obtained via a Schiff-base reaction between a new triamino-monomer (TABPB) and 2,5-divinylterephthalaldehyde, followed by the thiol-ene “click” reaction between 1,2-ethanedithiol and the vinyl groups. The COF-S-SH was characterized by FT-IR spectrum, energy-dispersive X-ray spectrum, 13 C MAS NMR spectrum, nitrogen adsorption–desorption isotherms, thermo-gravimetric analysis, scanning electron microscope, X-ray diffraction, and zeta potential. The new adsorbent showed high binding ability with the maximum adsorption capacities ( Q max ) of 150.2–255.8 mg/g for BTEX and 588.2 mg/g for Hg(II). The adsorbent also presented fast adsorption kinetics with rate constants of 0.01043–0.05002 g/mg/min for BTEX and 7.254 × 10 −4 g/mg/min for Hg(II). Moreover, the adsorbent had good binding selectivity for Hg(II) against common metal ions in water. The adsorbent also showed good simultaneous uptake ability and good reusability for BTEX and Hg(II), and it has been applied to simultaneously removing BTEX and Hg(II) in the simulated sewage with the removal efficiencies of 63.6, 82.1, 94.6, 95.3 and 94.1% for benzene, toluene, ethyl benzene, m-xylene and Hg(II), respectively. Especially, it can reduce the low-concentration Hg(II) in the simulated sewage to a level lower than the drinking water limit. Therefore, COF-S-SH can be used as an excellent adsorbent material for simultaneously removing BTEX and Hg(II) in from the produced water and wastewater in petroleum chemistry industries.
研究领域:
环境科学
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材料科学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2014
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IF 2.235
Dongju Wang,Hou Chen,Fujun Cao,Jinming Sun
Zinc powder was used as both reducing agent and supplemental activator for atom transfer radical polymerization via activators regenerated by electron transfer (ARGET ATRP) to prepare polyacrylonitrile (PAN). Zinc powder was found to be an excellent additional agent with better controlled behavior, higher monomer conversion, and faster polymerization rate in comparison with ascorbic acid (VC). The effects of catalyst, ligand, and initiator on polymerization rate and molecular weight of PAN were investigated in detail. The resulting PAN was modified and employed as an adsorbent for removal of metal ions. Compared with Cu(II) and Pb(II), the modified PAN showed an excellent adsorption performance toward Hg(II).
研究领域:
高分子化学
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环境科学
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DOI
高影响因子
Polymers
·
2023
·Vol. 15
·期 12
·2735
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IF 5
Qizhong Xiong,Lei Zhang,Zijun Zhu,Gang Xu,Jianyuan Jing,Weifeng Zhang,Chaochun Zhang,Xinxin Ye
Cellulose, a kind of polymer containing abundant functional groups, has widespread use in the adsorptive removal of environmental pollutants. An efficient and environmental friendly polypyrrole (PPy) coating approach is employed to modify the agricultural by-product straw derived cellulose nanocrystal (CNC) into excellent property adsorbents for removing the heavy metal ion of Hg(II). The FT-IR and SEM-EDS results demonstrated that PPy is formed on the surface of CNC. Consequently, the adsorption measurements proved that the obtained PPy-modified CNC (CNC@PPy) possesses a remarkably enhanced Hg(II) adsorption capacity of 1095 mg g−1, owing to a plentiful functional group of doped Cl element on the surface of CNC@PPy by forming Hg2Cl2precipitate. The results of the study suggest that the Freundlich model is more effective than the Langmuir model at describing the isotherms, while the pseudo-second order kinetic model is better suited to correlating with the experimental data compared to the pseudo-first order model. Further, the CNC@PPy exhibits an outstanding reusability, capable of maintaining 82.3% of its original Hg(II) adsorption capacity after five successive adsorption cycles. The findings of this work reveal a method to convert the agricultural by-product into high performance environmental remediation materials.Keywords:CNC;CNC@PPy;Hg(II) adsorption;agricultural waste
研究领域:
环境科学
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材料科学
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PubMed
高影响因子
RSC Advances
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2016
·Vol. 6
·期 18
·14916-14926
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IF 3.289
Qiugen Zhang,Jingyi Wu,Xubiao Luo
A novel magnetic ion-imprinted polymer (MIIP) with incorporated Fe3O4@SiO2 nanoparticles was synthesized via a surface imprinting technique using allylthiourea (ATU) as a functional monomer. The MIIP has an excellent saturation magnetization of 15.9403 emu g−1. Solution pH values had an immediate influence on the Hg(II) adsorption capacity with optimal removal occurring at pH 6. The adsorptivity of MIIP towards Hg(II) ions (78.3 mg g−1) was approximately twice that of a magnetic non-ion-imprinted polymer (39.5 mg g−1). The adsorption indicated that the adsorption mechanism closely agreed with a pseudo-second-order adsorption process, with a correlation coefficient (R2) of 0.998, which could be attributed to the soft acid–soft base interaction of Hg(II) and allylthiourea. The relative selectivity coefficients of MIIP for Hg(II)/Ni(II), Hg(II)/Cu(II), Hg(II)/Co(II) and Hg(II)/Cd(II) were 623, 355, 623 and 155, respectively. The recovery in rebinding capacity for Hg(II) was found to be decreased by only approximately 10.4% up to the 6th cycle, which suggests an excellent stability of MIIP. The application of MIIP in real samples shows a removal rate for Hg(II) of more than 99% to well below U.S. EPA mercury limits for wastewater, indicating that the MIIP has wide application prospects for Hg(II) removal in environmental water samples.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2017
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IF 4.9
Mingyang Sun,Guanghuan Cheng,Xinlei Ge,Mindong Chen,Cheng Wang,Liping Lou,Xinhua Xu
Stabilized iron sulfide (FeS) nanoparticles have been proven effective in the adsorption of Hg from the water environment. However, previous work with these nanoparticles determined that the separation from the treated water was difficult and time-consuming. In this study, nanoscale FeS-Fe 3 O 4 nanocomposites were firstly synthesized with chitosan as the stabilizer (CTO-MFeS). Then, the Hg adsorption capacity and mechanism were studied. Results showed that the size of the prepared nanoparticles was about 20 nm and the specific surface area was 21.3 m 2 /g. Hg removal by the CTO-MFeS nanoparticles involved both adsorption and precipitation. Further investigation with XPS showed that Hg 2 + was adsorbed on the surface of the CTO-MFeS nanoparticles and reacted with CTO-MFeS to form HgS and [Fe (1 − x) Hg x ]S. It was also found as pH decreased below 4, the adsorption capacity of CTO-MFeS was significantly reduced that might be due to the dissolving of Fe. Additionally, the presence of Cl − resulted in the transformation of Hg 2 + to HgClx 2-x (x = 1, 2, 3, 4) that competed with OH in solution for Hg 2 + and therefore inhibited the adsorption of Hg. Our findings provide additional information that may be useful for a theoretical basis for Hg treatment in water environment.
研究领域:
环境科学
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材料科学
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PubMed
高影响因子
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