INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Guili Wang,Chunxiao Li,Ming-Hsien Lee,Jiyong Yao
Currently, oxychalcogenides with mixed-anion groups that integrate the property advantages of oxides (wide optical band gap) and chalcogenides [strong second harmonic generation (SHG) response] through chemical substitution engineering have attracted widespread interest and are considered to be important candidates for infrared (IR) nonlinear optical (NLO) materials. Herein, the first Hg-based oxychalcogenide Sr2HgGe2OS6 with mixed anion [GeOS3] units has been successfully synthesized through a spontaneous crystallization method, which exhibits a favorable balance between the strong SHG response (0.7 × AgGaS2) and large optical band gap (2.9 eV). In addition, Sr2HgGe2OS6 shows high laser-induced damage threshold (LIDT, 2.1 × AgGaS2) as well as phase-matching (PM) performance. Theoretical calculations indicate that the Sr2HgGe2OS6 encompasses large birefringence of 0.128@2090 nm (3.3 × AgGaS2) and its SHG density mainly comes from [HgS4] tetrahedra and [GeOS3] units. This work not only demonstrates that Sr2HgGe2OS6 is a promising IR NLO material but also provides new ideas for the exploration of Hg-based oxychalcogenide IR NLO materials.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Jiarui Zhang,Bianyan He,Yubing Wang,Shanshan Li,Jiangtao Feng,Mingtao Li,Wei Yan
The development of novel high-capacity porous materials is critical to advancing the treatment of mercury-containing wastewater. In this study, two reticular poly(pyrrole methylene) adsorbent materials (PPB2E and PPD2E) were synthesized by a synchronous cross-linking method and successfully employed for Hg(II) adsorption in water. Their adsorption performance on Hg(II) in water was investigated. The results showed that PPB2E and PPD2E have large specific surface areas (535.43 m 2 /g and 523.23 m 2 /g, respectively) and are abundant microporous, with the molecular chains partially cross-linked and partially oxidized to form a conjugated structure. The adsorption of Hg(II) by the two adsorbents could reach equilibrium within 120 min, and the adsorption behavior followed the pseudo-second-order model. The adsorption isotherms were more in line with the Langmuir model, and the maximum adsorption capacities of PPB2E and PPD2E for Hg(II) were up to 1537.46 mg/g and 1511.94 mg/g (298 K, pH = 4), respectively. The two adsorbents exhibited excellent adsorption selectivity for Hg(II) in mixed metal salt solutions with good cycling stability. The primary adsorption mechanism of the synthesized materials for Hg(II) was jointly verified by characterization and DFT calculations: Hg(OH) 2 molecules were adsorbed by forming hydrogen bonds with pyrrole N and carboxyl O in the adsorbents. Compared with other metal ions, the materials have more active sites for Hg(II) adsorption, higher utilization, and easier formation of stable adsorption configurations, thus exhibiting highly selective adsorption.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Yingying Fang,Guangliang Liu,Ying Wang,Ligang Hu,Yong Liang,Yongguang Yin,Yong Cai,Guibin Jiang
Mercury (Hg) biogeochemical cycling involves redox transformations between Hg(0) and Hg(II), likely via a mercurous Hg(I) intermediate. Despite previously thought metastable, Hg(I) was found to exist stably in natural waters; yet, the redox behavior governing Hg(I) occurrence remains elusively studied. Here, we simulated an environmental Eh gradient (0.219–0.600 V, vs SHE) using noninterfering 1,4-benzoquinone and 1,4-hydroquinone as redox mediators, and demonstrate that Hg(I) redox transformations are strongly Eh-dependent. Hg(I) was stable at 0.302–0.339 V, contrasting significant oxidation (19–98%) at 0.369–0.600 V or reduction (81%) at 0.219–0.255 V. Speciation analysis and thermodynamic calculations confirm that varying proton level alters Hg(II) species abundance (HgHPO4, HgPO4–, and Hg(OH)2), driving this Eh-dependence. Specifically, HgHPO4/HgPO4– exhibits lower reduction potentials (to Hg(I), as Hg2(OH)2) than Hg(OH)2. Consequently, Hg(I) is subject to oxidation to HgHPO4/HgPO4– at 0.369–0.440 V (pH 6.0), while Hg(OH)2 preferentially undergoes stepwise reduction to Hg(I) and Hg(0) at 0.236–0.308 V (pH 7.5). Additionally, externally forced Hg(0) removal processes, e.g., purging used in conventional Hg(0) analysis, significantly affect Hg(I) transformations and enhance Hg reduction under reducing conditions, whereas natural degassing has negligible effects. This work provides valuable parameters for Hg redox thermodynamics and important implications for predicting Hg(I) occurrence in aquatic environments.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 5
·1-6
·
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.
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RSC Advances
·
2016
·Vol. 6
·期 89
·86428-86435
·
IF 3.289
Chunlai Wu,Guifen Zhu,Jing Fan,Jianji Wang
In this work, for the first time, neutral red functionalized Fe3O4@SiO2 was prepared, characterized and subsequently used for magnetic solid phase extraction of Hg(II) from environmental water samples followed by inductively coupled plasma-mass spectrometry determination. TEM images shows uniform decoration of SiO2 on the Fe3O4 surface (with a typical particle size of 220 nm). The FT-IR analysis indicates that neutral red was combined with the SiO2 surface by chemical bonds. Trace levels of Hg(II) can be extracted efficiently and selectively due to the electrostatic and coordinate interactions of Hg(II) and neutral red. Parameters affecting the quantitative recovery of Hg(II) were investigated, and the optimized values were 6.0, 25 mg, 60 min, and 5 mL of 1.0 mol L−1 HNO3 for pH value of the solution, amount of the extractant, equilibration time and volume, concentration of eluent, respectively. Under the optimized conditions, at Hg(II) concentrations as low as 2 ng mL−1, the recovery is >85%, and the enrichment factor is as high as 100. The commonly encountered ions show no interference with the extraction process. The material can be regenerated and reused at least ten times without loss of adsorption capacity (84 mg g−1). In addition, magnetic separation greatly simplifies the extraction procedure and filtration and/or centrifugation processes were avoided. The material was successfully applied for the separation and pre-concentration of low levels of Hg(II) in environmental water samples with satisfactory results.
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DYES AND PIGMENTS
·
2020
·
IF 4.613
Xiaotian Yuan,Yujiao Tu,Wei Chen,Zhiwei Xu,Yunlin Wei,Kunhao Qin,Qi Zhang,Yingying Xiang,Hongcai Zhang,Xiuling Ji
A highly photoluminescent small-size carbon dots (CDs) deriving ampicillin sodium were successfully obtained via one-step hydrothermal method . The prepared CDs showed uniform particle size and possessed good excitation-dependent characteristic. The dead bacteria and yeast cells could be selectively stained by the CDs, but the live ones not. It indicated that the CDs possessed a good potential for the live/dead bacteria and yeast differentiation. Cell and plant leaf imaging showed that the prepared CDs possessed low biotoxicity, excellent biocompatibility and multicolor fluorescence emission properties making it a good candidate for bioimaging application. The probe exhibited high selectivity and sensitivity to detect Hg(II) and 2,4-dinitrophenol (2,4-DNP), and excellent linear range of 0–50 μM for Hg(II) (R 2 = 0.9920) and 0–25 μM for 2,4-DNP (R 2 = 0.9919), with low detection limits of 33.40 nM and 13.44 nM for Hg(II) and 2,4-DNP, respectively. It revealed that dynamic quenching mechanism dominated in Hg(II) quenching the CDs fluorescent, while the quenching mechanism of 2,4-DNP detection belonged to the inner filter effect. The sensor was successfully applied to determine the Hg(II) and 2,4-DNP in real water samples. It shows that the fluorescent nanoprobe shows great promising potential for the detection of environmental pollutants.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 3
·649-657
·
IF 9.405
Xing Li,Yue Qi,Guozong Yue,Qianxun Wu,Yang Li,Meicheng Zhang,Xinghua Guo,Xiaofeng Li,Lijian Ma,Shoujian Li
A green and facile solvent- and catalyst-free method, without inert gas protection and/or mechanical grinding to synthesize an azine-linked covalent organic framework (ACOF) with high efficiency, was proposed for the first time. Characterization techniques and experimentations show that the as-synthesized ACOF has high crystallinity and superior physical and chemical stability and exhibits good adsorption performance for both radioactive heavy metal U(VI) and ordinary heavy metal Hg(II), with adsorption capacities of 169 mg g−1 for U(VI) and 175 mg g−1 for Hg(II), which makes the ACOF a potential adsorbent material for heavy metal removal and uranium recycling. Tautomerization between the enol-form and keto-form was verified in the structure of the ACOF which can be induced by the adsorption of metal ions and also affect the adsorption properties simultaneously. It was found that tautomerization from the enol-form to keto-form was promoted in the adsorption, which can be ascribed to the better coordination ability of CO in the keto-form towards the target metal ion, while the selectivity of the ACOF towards U(VI) increases with the decreasing solution pH and reaches 96.2% when the pH is 1.5, which is due to the tautomerization from the keto-form to enol-form under acidic conditions and the consequent size-matching effect. The study on tautomerization in solid materials is rarely reported and is of great importance for deep understanding of the relationship between material structures and properties. The synthesis strategy proposed in this paper provides references for the convenient, efficient and green synthesis of COFs.
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MICROCHEMICAL JOURNAL
·
2019
·
IF 3.206
Yajun Zhang,Xiaoliang Zeng,Xiaofang Jiang,Hanjiao Chen,Zhou Long
The cerium (Ce)-based UiO-66 metal-organic frameworks were employed for the first time as an effective catalyst for both oxidation and reduction. On one hand, selenium (Se)(VI) was efficiently photo-reduced to volatile species derived from the low lying of Ce 4f orbital and efficient generation of photo-electrons through the frameworks of UiO-66(Ce); on the other hand, the chromogenic substrate, 3, 3′, 5, 5′-tetramethylbenzydine (TMB), was oxidized based on the oxidase-like behavior of UiO-66(Ce) derived from the Ce 4+ /Ce 3+ spontaneous redox couple. The photo-reduced Se(VI) was determined by atomic fluorescence spectrometry , with a linear range of 5.0–200.0 μg/L − 1 , correlation coefficient of 0.998, and detection limit of 1.5 ng/mL − 1 obtained. The colorimetric sensing of mercury (Hg)(II) was accomplished based on the inhibition of TMB oxidation via Hg (II)-TMB interaction, with two linear ranges of 0.1–2.0 μM and 2.25–4.1 μM obtained, and a correlation coefficient of 0.993 and 0.995 obtained, respectively. The catalytic activity of UiO-66(Ce) was demonstrated to be satisfactory for both oxidation and reduction, which further explored the application of UiO-66(Ce) in the field of catalysis.
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MICROCHIMICA ACTA
·
2018
·Vol. 186
·期 1
·1-8
·
IF 5.705
Wang Yi-Wei,Liu Qiao,Wang Lixing,Tang Shurong,Yang Huang-Hao,Song Hongbo
A one-step reduction method was used for the preparation of stable graphitic carbon nitride-gold nanoparticles (g-C 3 N 4 -Au) nanocomposites from ultrathin g-C 3 N 4 nanosheets and chloroauric acid by using NaBH 4 as a reducing agent under ultrasonication. The nanocomposites were characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, UV-Vis absorption and fluorescence spectroscopy etc. The results revealed that the gold nanoparticles (AuNPs) are uniformly formed on the g-C 3 N 4 nanosheets. It is found that the peroxidase-like catalytic activity of this nanocomposite for the oxidation of 3,3′,5,5′-tetramethylbenzidine by H 2 O 2 to form a blue-colored product is strongly enhanced in the presence of Hg(II). Based on this phenomenon, a sensitive “turn-on” colorimetric assay for Hg(II) was developed that works at physiological pH values. Under optimal conditions, the absorption signal at 652 nm increases linearly with Hg(II) concentration in the range from 5 to 500 nM. A detection limit as low as 3.0 nM was achieved. This assay has excellent selectivity over other metal ions. It was successfully applied to the determination of Hg(II) in real water samples. The method is cost-effective, rapid, and allows for visual detection.
The nanocomposite composed of graphitic carbon nitride (g-C 3 N 4 ) and gold nanoparticles (g-C 3 N 4 -AuNPs) can catalyze tetramethylbenzidine (TMB) oxidation by H 2 O 2 to produce light-blue product (oxTMB). The peroxidase-like activity of g-C 3 N 4 -AuNPs can be greatly enhanced by Hg 2+ , thus increases the amount of the blue product formed.
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JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Yong Fu,Jinwen Jiang,Zhangpei Chen,Shaoming Ying,Jiwei Wang,Jianshe Hu
The toxic Hg(II) being released excessively into the water body from various sources has threatened the environment and human health. The aim of this study is to design a rapid and selective adsorbent, and propose an alternative way to dispose the spent adsorbent. To this end, a new material ( MAP ) was designed by inducing the polymerization of m -aminothiophenol onto MCM-41 (Mobil Composition of Matter) surface obtained using cheap diatomite as a silica source and modified by APTES ((3-aminopropyl) triethoxysilane), and the spent adsorbent was further converted into an active catalyst for acetophenone synthesis. The adsorption properties of the MAP were systematically explored under different parameters, and the corresponding results were analyzed based on different adsorption kinetic and isotherm models. The study found the removal rate and adsorption capacity of the MAP could reach 96.56% and 242.42 mg/g within 15 min. The coexisting cations showed little competition effect on the removal of Hg(II), and the adsorption capacities after five cycles did not obviously decrease. Kinetic study indicated that the adsorption data were well fitted to the pseudo-second-order model, and the adsorption equilibrium data followed the Langmuir model. After adsorption studies, the Hg(II)- MAP was used as a catalyst in the reaction of phenylacetylene to acetophenone with high yield of 97.01%. This work not only provides a rapid and selective adsorbent for removal of Hg(II) ions, but also opens a novel avenue for reusing the toxic spent adsorbent for catalytic application.
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MICROCHIMICA ACTA
·
2015
·Vol. 182
·期 13
·2251-2258
·
IF 3.741
Wang Minghua,Zhang Shuai,Ye Zihan,Peng Donglai,He Linghao,Yan Fufeng,Yang Yanqin,Zhang Hongzhong,Zhang Zhihong
Multilayered reduced graphene oxide (rGO) was functionalized with amino groups by treatment with nitrogen plasma. Raman spectroscopy showed plasma treatment not to substantially alter the chemical structure of rGO and that a wide range of functional nitrogen groups is evenly incorporated into the carbon lattice. The amino-modified rGO was used to design an electrochemical biosensor in which a DNAzyme, substrate DNA and Pb(II) and Hg(II) binding DNA were immobilized on the amino-rGO placed on a gold electrode. The high concentration of amino groups and the rough surface of the rGO favor DNA immobilization. Heavy metal ions are bound to the surface via specific interaction between DNA and the two ions which are detected by electrochemical impedance spectroscopy at a potential of 0.2 V (vs. Ag/AgCl). The detection limits for Pb(II) and Hg(II) are as low as 7.8 and 5.4 pM, respectively, and the analytical ranges extend from 0.01 to 100 nM. The sensor is highly specific and stable and therefore represents a highly promising tool for use in environmental monitoring.
A nanofilm of reduced graphene oxide was first modified with amino groups by treatment with nitrogen plasma. A special DNA was then anchored to the surface to obtain a biosensor for simultaneous detection of Pb(II) and Hg(II). The sensor has detection limits as low as 7.8 and 5.4 pM and is highly selective.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2015
·
IF 4.097
Zhihong Zhang,Xiaoming Fu,Kunzhen Li,Ruixue Liu,Donglai Peng,Linghao He,Minghua Wang,Hongzhong Zhang,Liming Zhou
A novel DNA-modified nanocomposite of three-dimensional reduced graphene oxide and chitosan particles (CS@3D-rGO@DNA) was prepared by one-step method and used as a new electrochemical biosensing strategy to detect Hg 2+ in drinking water . This biosensor was fabricated by the chemical coordination of T-Hg 2+ -T between the T-rich oligonucleotide strands contained in the as-prepared CS@3D-rGO@DNA nanocomposite and Hg 2+ , thereby varying the electrochemical signals. The developed electrochemical biosensor exhibited high sensitivity toward the determination of Hg 2+ with a low detection limit of 0.016 nM, ranging from 0.1 nM to 10 nM. This novel biosensor also showed high selectivity, good stability, and repeatability. Hence, this proposed CS@3D-rGO@DNA-based electrochemical strategy is feasible and may offer a simple, rapid, cost-effective, highly selective, and sensitive method for Hg 2+ quantification.
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