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CHEMOSPHERE · 2021 · IF 7.086

Kinetics, isotherm and chemical speciation analysis of Hg(Ⅱ) adsorption over oxygen-containing MXene adsorbent

Xiaolan Hu,Changhong Chen,Dawei Zhang,Yingwen Xue

A facile method was used to prepare two-dimensional MXene for the treatment of heavy metal ions in wastewater. The adsorbent has good selectivity for the adsorption of Hg (Ⅱ) in mixed divalent cationic metal solutions due to a large number of oxygen-containing functional groups on the surface of the material. The adsorption of mercury was tested using mercuric chloride and mercury nitrate solutions. The Langmuir maximum adsorption capacity of the adsorbent at a pH of 5.0 and a temperature of 30 °C is 1057.3 mg/g (mercuric nitrate) and 773.29 mg/g (mercuric chloride), respectively. The adsorbent also maintains a high adsorption capacity at low pH (pH = 2.0). The removal rate of mercury-containing wastewater within 100 mg/L is nearly 100%. The chemical species of Hg-containing ions at different pH and temperatures was studied. It was found that the adsorbent could maintain a high adsorption capacity for different forms of Hg-containing ions.

CAS / MDL: 7631-99-4 196506-01-1
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TEXTILE RESEARCH JOURNAL · 2020 · IF 1.926

Characterization of a versatile glycoside hydrolase Cel5M from Pectobacterium carotovorum HG-49 for ramie degumming

Yawei Wang,Yun Bai,Tong Shu,Pei Fan,Huashan Zhang,Ossi Turunen,Hairong Xiong,Longjiang Yu

A novel versatile glycoside hydrolase Cel5M was identified from Pectobacterium carotovorum and used in ramie degumming. The full-length Cel5M (GenBank: MH544226) containing the catalytic domain Cel5MD and its carbohydrate-binding module (CBM3) were expressed in E. coli. Both Cel5M and Cel5MD showed a broad substrate spectrum cleaving konjac glucomannan (KGM), carboxymethylcellulose (CMC) and oat spelt xylan. The optimal temperature of Cel5MD was 55oC with CMC and KGM, whereas the optimum temperature of Cel5M was 65oC with KGM and 60oC with CMC. The improved thermal activity with KGM was probably reflected also in the much lower Km with KGM than with CMC, indicating stronger binding of the full-length enzyme with KGM. Both enzymes were highly stable over a broad pH range from pH 5.0 to 9.0 with KGM. The use of the Cel5M enzyme together with the wild-type P. carotovorum HG-49 strain showed significant improvement when compared to using the mere strain HG-49 for application in ramie degumming. Moreover, the whole P. carotovorum Cel5M gene was over-expressed in P. carotovorum HG-49 itself to improve the ramie-degumming capacity. Altogether, this study indicates that in situ production of processing enzymes could be utilized in the textile industry.

CAS / MDL: 9000-30-0
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Recyclable DNA-Derived Polymeric Sensor: Ultrasensitive Detection of Hg(II) Ions Modulated by Morphological Changes

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.

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JOURNAL OF APPLIED POLYMER SCIENCE · 2023 ·Vol. 141 ·期 4 ·e54853 · IF 3

Fluorescent naphthalimide containing polyurethanes for the detection and removal of Hg2+/Hg+ and Fe3+ ions

Meng Xie,Ke Yang,Yuye Wang,Xinjian Cheng

Heavy metal (HM) pollution is getting worse with the society progress. Identification and separation of HM ions are urgent issues in environmental protection and social development. In this work, 4-bromo-1,8-naphthalic anhydride was first reacted with amino-propylene glycol to synthesize naphthimide fluorophores bearing two hydroxyl groups. And then, –Br was substituents by 8-mercaptoquinoline, 2-mercaptoimidazole, and 4-mercaptopyridine, respectively. Eventually, it was reacted with 1,5-naphthalene diisocyanate (NDI) to synthesize fluorescent polyurethane (PU) films through the reaction between –OH and –NCO. It is found that the PU film not only has a specific identification ability to Hg 2+ /Hg + and Fe 3+ ions, but also can efficiently remove Hg 2+ /Hg + and Fe 3+ ions through adsorption. In addition, selective identification by fluorescence quenching was investigated. It is due to the photoinduced electron transfer mechanism (PET). Furthermore, the lowest detection limits for Fe 3+ , Hg 2+ , and Hg + were 6.0 × 10 −7 M, 4.7 × 10 −7 M, and 9.7 × 10 −7 M, respectively, which reflected the sensitivity of the probe and made it fluorescence probes. The three fluorescent small molecules were incorporated into PU, which not only retain their identification function, but also serve the purpose of adsorption and separation of HM ions.

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CHEMICAL ENGINEERING RESEARCH & DESIGN · 2023 · IF 3.9

Hypophosphorous acid functionalized nanoporous silicon for selective adsorption of Hg(II) in industrial waste water

Huizhen Sun,Yi Li,Xiumin Chen,Xiuhua Chen,Shaoyuan Li,Wenhui Ma,Kaixin Fu

The recycling of diamond wire cutting silicon waste (DWCSW) and the removal of heavy metal ions are very important for human life. Therefore, it is a promising method to improve the selective removal of heavy metal ions by etching and modifying organic functional groups for DWCSW. In this study, a new adsorbent PA-TEPA-GTS-NPSi was synthesized by Cu-assisted chemical etching and modified with 3-glycine dioxy-propyl trimethoxy-silane (3-GTS), tetraethylpentenediamine (TEPA) and hypophosphorous acid (H 3 PO 2 ) for selective adsorption Hg(Ⅱ). PA-TEPA-GTS-NPSi showed excellent adsorption performance on Hg(Ⅱ), with adsorption capacity of 112.8 mg/g (pH=2.0, adsorption time=120 min). The pseudo-second-order model and Langmuir model can better describe the adsorption process , which proving that the adsorption process is chemisorption . The adsorption mechanism of Hg(Ⅱ) was studied by X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT). It was proved that the adsorption process was mainly caused by the strong adsorption between P and Hg(Ⅱ) in the phosphorus groups on the surface of PA-TEPA-GTS-NPSi adsorbent. Compared with other hypophosphorous acid functionalized adsorbents, the adsorption performance of the adsorbent is at a medium level, but it can effectively recycle DWCSW while removing heavy metal ions.

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Progress in Natural Science-Materials International · 2023 · IF 4.7

Recyclable thiol-modified Zr-based MOFs/hydrogel composite beads for effective removal of Hg (II)

Xuechun Wang,Zeming Dai,Xuan Zhou,Hao Chen,Yu Cao,Jianhua Hou,Xiaozhi Wang

In general, majority of MOFs are powder, which limit their applications. In this study, the highly stable Zr-based MOF-808 and its thiol-modified MOF-808-SH were selected as precursors, and then they were wrapped by sodium alginate hydrogel via a dripping strategy. Based on these, MOF/hydrogel composite beads (Alg-MOF-808, Alg-MOF-808-SH) with 3D network structure were prepared successfully. Due to its excellent adsorption properties and easy recovery, they were employed as effective environmental functional materials for the adsorption of Hg (II). The adsorption capacities of Hg (II) were 170.52 ​mg‧g −1 and 221.73 ​mg‧g −1 respectively and they can achieve adsorption equilibrium in a short time. The adsorption stability of Alg-MOF-808-SH was studied at different pH as well. In addition, the removal efficiency of composite beads for Hg (II) was almost unaffected by other coexisting ions, displaying good adsorption selectivity. Furthermore, the removal efficiency only decreased by 10.4% after 5 cycles, indicating that the as-prepared materials have high recycling efficiency. The results demonstrated that the MOF/hydrogel composite beads have a certain application potential for mercury removal in actual wastewater.

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Chemosensors · 2023 ·Vol. 11 ·期 6 ·347 · IF 4.2

Recyclable Multifunctional Magnetic Fe3O4@SiO2@Au Core/Shell Nanoparticles for SERS Detection of Hg (II)

Chao Liu,Hui Wang,Shengmin Xu,Hongbao Li,Yilin Lu,Chuhong Zhu

Mercury ions can be enriched along the food chain and even low concentrations of mercury ions can seriously affect human health and the environment. Therefore, rapid, sensitive, and highly selective detection of mercury ions is of great significance. In this work, we synthesized Fe3O4@SiO2@Au three-layer core/shell nanoparticles, and then modified 4-MPy (4-mercaptopyridine) to form a SERS sensor. Mercury ions in water can be easily captured by 4-MPy which were used as the reporter molecules, and the concentration of mercury ions can be evaluated based on the spectral changes (intensification and reduction of peaks) from 4-MPy. After the mercury ion was combined with the pyridine ring, the peak intensity at 1093 cm−1increased with the concentration of mercury ion in the range of 10 ppm–1 ppb, while the Raman intensity ratio I (416 cm−1)/I (436 cm−1) decreased with the increase of mercury ion concentration. This magnetically separatable and recyclable SERS sensor demonstrates good stability, accuracy, and anti-interference ability and shows the potential to detect actual samples. Furthermore, we demonstrate that the probe is applicable for Hg2+imaging in macrophage cells.Keywords:core/shell nanoparticles;4-pyridinethiol;surface-enhanced Raman spectroscopy (SERS);Mercury (II) ion;Raman cell imaging

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ACS Applied Nano Materials · 2023 · IF 5.9

Controllable Fabrication of Hg–Pd–PdO Heterostructures as Efficient Peroxidase Mimics for Carcinoembryonic Antigen Detection

Lulu Kong,DeZhu Chen,Xiaolong Zhang,Lin Zhou,Yongming Deng,Shaohua Wei

The growth of oxides on the surface of noble metals and the introduction of alloys are effective methods to enhance the catalytic activity of noble metals. However, the fabrication of noble metal oxides always involves harsh experimental conditions and the oxidation degree could not be controlled. Herein, a simple, fast, and controlled Pd oxidation method by mixing Hg2+ and Pd nanosheets (PdNSs) under mild conditions to form PdxHgy(PdO)z (PHOs) was reported, which consists of the Pd–Hg alloy and PdO. The density functional theory (DFT) calculation and experiment results proved that the Hg atom incorporation promotes the nearby Pd–Pd bond breaking, initiating a cascade of PdO generation. More precisely, 1 Hg atom incorporation induced ∼8 Pd atom oxidation, ensuring that the oxidation degree of Pd could be easily controlled by adjusting the ratio of Hg2+ and PdNS. As a peroxidase-mimicking nanozyme, the PHO affinity for its substrate could be 21.7- and 123.6-fold greater than that of the PdNS and the natural peroxidase (HRP), respectively. For the colorimetric immunoassay of carcinoembryonic antigen (CEA) detection, PHO has an ultralow detection limit of 1.33 pg mL–1, which is ∼8.6 and ∼282 times lower than that of the PdNS and the natural HRP, respectively.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2017 · IF 4.233

Three-dimensional molybdenum disulfide/graphene hydrogel with tunable heterointerfaces for high selective Hg(II) scavenging

Yu-Ting Zhuang,Xiao Zhang,Dan-Hua Wang,Yong-Liang Yu,Jian-Hua Wang

A hierarchical and hybridized hydrogel with rational structure and composition as adsorbent possesses a series of distinct advantages, e.g., fast ion diffusion, high selectivity and good stability. Herein, a novel three-dimensional (3D) molybdenum disulfide (MoS 2 )-reduced graphene oxide (rGO) hydrogel with two-dimensional heterointerfaces is fabricated by an eco-friendly one-pot hydrothermal method. The heterointerfacial area could be readily tuned by the regulation of MoS 2 /rGO ratio, in order to improve the adsorption capacity and selectivity. The 3D MoS 2 -rGO hydrogel with 70 wt% MoS 2 shows high selectivity for Hg(II) ions, with a distribution coefficient value (K d ) of 7.49 × 10 6  mL g −1 even in the presence of other coexisting ions. More attractively, the free-standing and flexible 3D MoS 2 -rGO hydrogel can be used as a column-packed device, providing an efficient pathway for the fast removal of 80 mg L − 1 Hg(II) within 7 min to achieve a tolerable concentration of < 2 μg L −1 in 30 mL water with 5 mg of 3D MoS 2 -rGO hydrogel. Considering that the direct-contact adsorption is more efficient than oscillating adsorption, the 3D MoS 2 -rGO hydrogel as nanobuilding block shows a promising potential for cleaning the point-of-use water.

CAS / MDL: 56570-89-9
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APPLIED SURFACE SCIENCE · 2015 · IF 2.711

Comparative study of Hg(II) adsorption by thiol- and hydroxyl-containing bifunctional montmorillonite and vermiculite

Lytuong Tran,Pingxiao Wu,Yajie Zhu,Shuai Liu,Nengwu Zhu

A novel approach to prepare adsorbents for Hg(II) uptake from aqueous media based on the grafting of dimercaprol (BAL), containing thiol and hydroxyl groups, onto the natural montmorillonite and vermiculite was investigated concerning the evaluation of the adsorption capacity. The kinetic study showed that the adsorption process abided by pseudo-second-order model. The adsorption behavior of Hg(II) onto the obtained samples fitted well with Langmuir isotherm model, exhibiting an enhanced maximum adsorption capacity of 8.57 and 3.21   mg   g −1 for BAL-Vm and BAL-Mt, respectively. The feasibility of Hg(II) uptake onto the the samples was studied thermodynamically and the calculated coefficients such as Δ H , Δ S and Δ G indicated a physical and spontaneous process. The pH values and coexisting cations had a great influence on Hg(II) removal, confirming the optimal pH value of 4.0–5.0 and the negative correlation between the ionic strength and the adsorption capacity of Hg(II). In general, BAL-Vm possessed a higher efficiency of Hg(II) uptake than BAL-Mt, contrary to that of the pristine clays. The pristine and functionalized materials were investigated by XRD, FTIR, BET, SEM and zeta potential analysis to gain in-depth insight into the structure and surface morphology. The results showed that BAL was successful grafted on montmorillonite and vermiculite surface, providing plentiful adsorption sites as chelating ligands. The mechanisms of Hg(II) adsorption on these samples could be further explained as ion exchange and electrostatic attraction for Vm and Mt, and formation of complexes for BAL-Vm and BAL-Mt.

CAS / MDL: 59-52-9
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SENSORS AND ACTUATORS B-CHEMICAL · 2016 · IF 4.758

Facile fabrication of zinc phosphate-based nanocomposites for high-performance electrochemical sensing of Hg(II)

Linghao He,Shuai Zhang,Minghua Wang,Donglai Peng,Fufeng Yan,Zhihong Zhang,Liming Zhou

Two novel nanocomposites of zinc phosphate [Zn 3 (PO 4 ) 2 ] and Hg 2+ -targeted DNA [Zn 3 (PO 4 ) 2 @DNA] and Zn 3 (PO 4 ) 2 and multi-wall carbon nanotubes (MWCNTs) modified with Hg 2+ -targeted DNA [Zn 3 (PO 4 ) 2 @MWCNTs-DNA] were fabricated by the assembly of Hg 2+ -targeted DNA strands with Zn 2+ ions. Two as-prepared nanocomposites were subsequently used as electrochemical biosensors for sensitively detecting Hg 2+ due to the combination effect of the formation of T–Hg 2+ –T coordination between DNA strands and Hg 2+ and the direct adsorption of Hg 2+ onto porous nanocomposites. In comparing with Zn 3 (PO 4 ) 2 @DNA nanocomposite, the crystallization degree of Zn 3 (PO 4 ) 2 @MWCNTs-DNA was improved due to the presence of MWCNTs, which further enhance electrochemical activity of the nanocomposite. As a result, Zn 3 (PO 4 ) 2 @MWCNTs-DNA nanocomposite-based electrochemical biosensor showed a higher sensitivity toward Hg 2+ detection in aqueous solution than Zn 3 (PO 4 ) 2 @DNA-based biosensor. It showed a detection limit of 0.071   nM within the range of 0.1–50   nM of the concentration of Hg 2+ . This newly developed biosensor also presented excellent selectivity, repeatability, and applicability in Hg 2+ detection. Therefore, the fabricated Zn 3 (PO 4 ) 2 -based nanocomposite using this novel strategy showed their considerable potential use in water or environmental treatment.

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Journal of Materials Chemistry A · 2024 · IF 10.7

Water-insoluble polyethyleneimine adsorbents for the high-efficiency removal of Hg(II) from aqueous solution

Xiaosai Hu,Haoran Cao,Man He,Junrui Miao,Yanyan Jin,Hongming Lv

Polyethyleneimine (PEI), with an abundance of amino groups, demonstrates a strong affinity for heavy metal ions, thus emerging as a promising candidate for applications in wastewater treatment. However, the inherent water solubility of PEI limits its direct use for the remediation of heavy metals. Contrary to the previous synthetic approaches that employed PEI solely as a surface modifier, the present work utilizes the PEI polymer as the fundamental matrix for the development of water-insoluble polyethyleneimine derivative adsorbents (PAPEI). This innovative method eliminates the need for additional solid substances, enabling the effective elimination of Hg(II) from aqueous solutions. PAPEI adsorbents achieved a high adsorption capacity of 1832 mg g−1 for Hg(II) with a good selectivity (distribution coefficient Kd = 3.2 × 104 mL g−1). The adsorption process between the PAPEI adsorbents and Hg(II) was primarily attributed to chelation affinity. This work proposed a straightforward approach for designing PAPEI adsorbents that can efficiently remove Hg(II) from aqueous environments.

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