JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Junlei Zhang,Wei Zhao,Shanshan Wu,Renli Yin,Mingshan Zhu
Advanced oxidation processes (AOPs) based on heterogeneous catalytic activated peroxymonosulfate (PMS) have been becoming alternatives to conventional wastewater treatment technologies to directly degrade chemical contaminants. To build dual/multi redox cycles of different metal ions may be an effective means for better PMS activation. Herein, this study designed Mn 3 O 4 /CuBi 2 O 4 with dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) to activate PMS for efficiently decomposing and mineralizing diclofenac sodium (DCF). Under optimal reaction conditions, DCF (50 mg/L) was degraded totally within 10 min, and TOC removal rate reached up to 74.3%. The possible mechanism of PMS activation by Mn 3 O 4 /CuBi 2 O 4 was proposed, wherein dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) on Mn 3 O 4 /CuBi 2 O 4 effectively facilitated PMS activation to generate · O 2 − , 1 O 2 , SO 4 · − and · OH, which was responsible for DCF degradation. Moreover, combined with degraded products detected by high resolution liquid chromatography coupled to mass spectrometry and corresponding toxic assessment results, the possible degradation pathways of DCF were proposed and the relative toxicity of degraded products was evaluated. This work may be useful for developing stronger heterogeneous activators of PMS to construct more efficient AOPs for purifying wastewater.
研究领域:
环境科学
·
化学工程
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 8
·3936-3944
·
IF 3.3
Binxiong Guang,Yiwei Zhang,Yahui Xiao,Miaojun Su,Yong Liu
To bridge transition metal complexes and heterogeneous catalysts for allylic oxidation of cyclohexene to 2-cyclohexene-1-one with O2 under mild conditions, Cu(II) coordinated N-bearing heteropolyacid-based poly(ionic liquid)s (Cu-PDVD-PW) were herein synthesized as novel heterogeneous catalysts. The physicochemical properties of the catalysts were investigated by BET, TG, XPS, FT-IR and SEM/EDS analysis. The results indicated that the as-prepared Cu-PDVD-PW catalyst inherited appreciable mesopores and excellent thermal stability from the N-bearing poly(ionic liquid)s, which could increase the mass transfer rate and provide more accessible active sites. Significantly, the Cu2+ cations were homogeneously and stably coordinated on the N-bearing poly(ionic liquid)s, which greatly improved the catalytic performance for cyclohexene oxidation toward 2-cyclohexene-1-one with O2 under mild conditions. Specifically, the 3% Cu-PDVD-PW catalyst exhibited 75.9% conversion of cyclohexene with a selectivity towards 2-cyclohexene-1-one of 45.5% and no activity loss within five cycles under the optimum reaction conditions.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Shiwei Xie,Chang Li,Hui Zhan,Wei Shao,Yuanxin Zhao,Peng Liu,Peng Liao
Fe-based replacement and precipitation are promising methods for removal of copper ethylenediaminetetraacetic acid (Cu(II)-EDTA) but are limited by the necessity of controlling pH and dissolved oxygen. The details of the decomplexation mechanism also remain unclear. The present work investigated an anoxic iron electrocoagulation process capable of automatically modulating anoxic conditions and solution pH during exposure to air and thus promoting the rapid and thorough decomplexation of Cu(II)-EDTA. Dissolved Fe (II), rather than Fe(II)-bearing minerals, was found to be primarily responsible for the reduction of Cu(II)-EDTA to Cu(I)-EDTA and for the subsequent replacement reaction to generate free Cu(I) ions within the initial pH range of 2–7. The Cu(I) was primarily precipitated as Cu 2 O on the surface of green rust and magnetite as the pH was increased. The aeration of these Fe-containing precipitates released free Cu(I) ions instead of chelated Cu into solution, allowing for recycling of the Cu. This release of Cu(I) was likely induced by the pH decrease during aeration. This study provides important insights regarding the reductive decomplexation of chelated Cu(II) and the recovery of Cu via anoxic iron electrocoagulation, which is a promising green approach to recycling Cu from wastewater.
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高影响因子
RSC Advances
·
2021
·Vol. 11
·期 12
·6699-6708
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IF 3.361
Mei Li,Xiaojuan Xia,Shuang Meng,YuChan Ma,Tong Yang,Yunhui Yang,Rong Hu
In this paper, a novel sandwich immunosensor based on a toluidine blue (Tb) loaded metal organic framework (Cu(II)-HKUST-1/Tb) as the signal element and a nitrogen-doped 3D carbon nanostructure as the electrode substrate was constructed for the detection of C-reactive protein (CRP). Tb as an electrochemically active agent usually forms a polymer by aggregation in the solvent, causing a poor electrochemical response. Therefore, in order to overcome this obstacle, Cu(II)-HKUST-1 with a porous nanostructure and large specific surface area as a carrier could adsorb a large number of Tb molecules on its surface to improve its electrochemical performance. In addition, the high electron transfer efficiency of the N-doped bamboo-like carbon nanotubes (CoFe/N-GCT) improves the sensitivity of the biosensor. Differential pulse voltammetry (DPV) was used to detect the current signal of Tb at −0.2 V. The current response increased with the increase in concentration of CRP, ranging from 0.5 to 200 ng mL−1. The detection limit is 166.7 pg mL−1 (S/N = 3). Moreover, the proposed biosensor can be applied in real serum sample detection. It has potential applications in the field of biomedicine assays.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Haize Su,Weipeng Qiu,Tianren Deng,Xiaoling Zheng,Hong Wang,Peng Wen
Efficient removal of contaminants, like heavy metal ions and dyes, from wastewater by eco-friendly and low-cost adsorbent is highly desirable. Herein, a green aerogel was prepared using sodium alginate/carboxylated chitosan/montmorillonite (MSC-P) as the basic framework, followed by polyethyleneimine functionalized and Ca 2+ post-crosslinking. The multi-crosslinked aerogel exhibited the excellent adsorption capacity towards methylene blue (MB), Congo red (CR) and Cu(II), with the q m being 723.97 mg/g, 1573.21 mg/g and 203.99 mg/g, respectively. The mathematical model suggested that the adsorption process for MB fitted pseudo-first-order kinetics model better, whereas the CR and Cu (II)’s adsorption process were conformed to pseudo-second-order kinetics model. Moreover, the adsorption isotherm for three contaminants could be well described by Langmuir model, suggesting that the adsorption process was spontaneous and mainly controlled by monolayer coverage. Moreover, MSC-P aerogel exhibited good reusability as the removal efficiencies for MB and Cu(II) were 85.16 % and 51.4 % after ten cycles of adsorption–desorption, respectively. Importantly, it possessed considerable simultaneous removal ability for binary system mixed dyes. In combination of FTIR analyses, it was found that electrostatic attraction, hydrogen bonding, coordination and cation exchange were the main adsorption mechanisms involved. Therefore, the as-prepared aerogel can be considered as a promising adsorbent for the treatment of wastewater.
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 4
·1-8
·
IF 5.705
Shao Hong,Xu Dan,Ding Yadan,Hong Xia,Liu Yichun
The authors describe an “off-on” colorimetric and fluorometric assay for the determination of Cu(II). It is based on the use of upconversion nanoparticles (UCNPs) of type NaYF 4 :Yb(III),Er(III) that were functionalized with branched polyethylenimine (BPEI). A color change from colorless to blue occurs within 2 s after addition of Cu(II) to a solution of the modified UCNPs. The color change can be visually detected at Cu(II) concentrations down to 80 μM. The upconversion fluorescence of the modified UCNPs, measured at excitation wavelength of 980 nm, is reduced due to the predominant inner filter effect caused by the formation of the BPEI-Cu(II) complex. Normalized fluorescence intensity drops linearly in the 50 nM to 10 μM Cu(II) concentration range, and the fluorometric detection limit is 45 nM. Both the color and the fluorescence are recovered on addition of EDTA. Excellent selectivity over other metal ions and anions is achieved.
Upconversion nanoparticles of type NaYF4:Yb,Er were functionalized with branched polyethylenimine (UCNP/BPEI) and used in an “off-on” colorimetric and fluorometric assay for Cu(II). The upconversion fluorescence is selectively quenched on addition of Cu(II), and this is accompanied by a rapid colorless-to-blue color switch. The colorimetric changes and quenched fluorescence can be reversed by adding EDTA.
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MICROCHIMICA ACTA
·
2017
·Vol. 184
·期 12
·4731-4740
·
IF 4.58
Lu Zhiwei,Zhang Junjun,Dai Wanlin,Lin Xueni,Ye Jiaping,Ye Jianshan
The authors report on a disposable sensor for the differential pulse anodic stripping voltammetric (DPASV) determination of the ions Zn(II), Pb(II) and Cu(II). Simultaneous detection is accomplished by using a screen-printed carbon electrode (SPCE) co-modified with an in-situ plated bismuth (Bi)) film and gold nanoparticles (AuNPs). The synergistic effect of the Bi film, and the large surface and good electrical conductivity of the AuNPs strongly assist in the co-deposition of the three ions. Four well-defined and fully separated anodic stripping peaks, at 540 mV for Zn(II), 50 mV for Pb(II), 140 mV for Bi(III) and 295 mV for Cu(II), all vs. Ag/AgCl, can be seen. The modified SPCE was characterized by scanning electron microscopy, X-ray diffraction, cyclic voltammetry and electrochemical impedance spectroscopy. Under the optimized conditions, the sensor has a good response to these ions. The detection limits (at an S/N ratio of 3) are 50 ng·L −1 for Zn(II), 20 ng·L −1 for Pb(II), and 30 ng·L −1 for Cu(II). The method was applied to the determination of the 3 ions in spiked lake water samples.
Schematic of screen-printed carbon electrode (SPCE) co-modified with a bismuth film and gold nanoparticles for electrochemical simultaneous determination of Zn(II), Pb(II) and Cu(II) by differential pulse anodic stripping voltammetric (DPASV).
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2015
·Vol. 16
·期 7
·14464-14476
·
IF 2.862
Jing Wei,Lu Han,Jing Song,Mengfang Chen
The objectives of this study were to evaluate the binding behavior of Cu(II) and Eu(III) with water extractable organic matter (WEOM) in soil, and assess the competitive effect of the cations. Excitation-emission matrix (EEM) fluorescence spectrometry was used in combination with parallel factor analysis (PARAFAC) to obtain four WEOM components: fulvic-like, humic-like, microbial degraded humic-like, and protein-like substances. Fluorescence titration experiments were performed to obtain the binding parameters of PARAFAC-derived components with Cu(II) and Eu(III). The conditional complexation stability constants (logKM) of Cu(II) with the four components ranged from 5.49 to 5.94, and the Eu(III) logKMvalues were between 5.26 to 5.81. The component-specific binding parameters obtained from competitive binding experiments revealed that Cu(II) and Eu(III) competed for the same binding sites on the WEOM components. These results would help understand the molecular binding mechanisms of Cu(II) and Eu(III) with WEOM in soil environment.Keywords:water extractable organic matter;copper;europium;excitation-emission matrix;parallel factor analysis
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高影响因子
Journal of Materials Chemistry B
·
2019
·Vol. 8
·期 5
·919-927
·
IF 5.047
Minghui Zan,Cong Li,Daoming Zhu,Lang Rao,Qian-Fang Meng,Bei Chen,Wei Xie,Xingwang Qie,Li Li,Xiaojiao Zeng,Yirong Li,Wen-fei Dong,Wei Liu
Copper ions (Cu2+) and L-cysteine (L-Cys) in the human body always play critical roles in various physiological processes, while abnormal Cu2+ and L-Cys concentrations in the biological system lead to many diseases. In this manuscript, Si-doped carbon dots (Si-CDs) with near-infrared fluorescence were designed for the detection of Cu2+ and L-Cys through the fluorescence “on–off–on” mode. The carbon dots exhibited not only excellent optical merits including good stability against photobleaching and high chemical stability, but also superior biological compatibility. Interestingly, due to the abundant amino groups distributed on the surface of Si-CDs, they could bind to copper ions to form cupric amine complexes and then quench the fluorescence of Si-CDs due to an electron transfer process. In addition, upon the addition of L-Cys, the FL intensity of Si-CDs could be effectively recovered accompanied with complexation between Cu2+ and the functional groups in L-Cys, due to which Cu2+ was removed from the surface of Si-CDs. Notably, as far as we know, these are the first red-emitting carbon dots for copper ion and L-Cys assays in water samples and human plasma samples. Furthermore, this strategy was successfully applied to the determination of Cu2+ and L-Cys in living systems, demonstrating great practicability in biomedical applications.
研究领域:
分析化学
·
生物医学工程
·
材料科学
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JOURNAL OF COORDINATION CHEMISTRY
·
2021
·
IF 1.751
Yan Zhao,Xianying Duan,Guangguang Zhang,Meilin Wei
Two proton-conductive and luminescent organic-inorganic hybrid materials, {[Cu(II)(bhmbpy)(H2O)(Cl)0.5(CH3CN)]2[PW(VI)10W(V)2O39]}·4H2O(1) and {H2[Cu(I)(bhmbpy)2(Cl)Cu(I)(bhmbpy)2][PW12O40]}·7H2O (2) (where bhmbpy is bis(hydroxymethyl)-2,2′-bipyridine), were synthesized at room temperature. The two products were characterized by infrared spectroscopy, X-ray single-crystal diffraction, X-ray powder diffraction, elemental and thermogravimetric analyses. The proton conductivities and luminescence of 1 and 2 were studied by using alternating-current impedance spectroscopy and luminescence spectroscopy, respectively. X-ray diffraction analysis revealed that 1 includes a decorated polyanion chain {[Cu(II)(bhmbpy)(H2O)(Cl)0.5(CH3CN)]2[PW(VI)10W(V)2O39]}n and forms a three-dimensional network structure depending on short Cl…Cl contacts and hydrogen-bonding interactions. X-ray diffraction analysis revealed that 2 includes a butterfly-like bi-nuclear copper cluster unit with a Cl-bridge, [Cu(I)(bhmbpy)2(Cl)Cu(I)(bhmbpy)2]+, and forms a three-dimensional network structure depending on hydrogen-bonding interactions. [PW12O40]3– anions fill in the network based on hydrogen-bonding and electrostatic interactions. In them, the bhmbpy acts as a bidentate nitrogen donor ligand in the chelating fashion to coordinate with the Cu(II) center in 1 and the Cu(I) center in 2. The bhmbpy in 2 successfully constrains the Cu(I) within a rigid environment in a tetragonal-pyramidal geometry. The two compounds exhibit good proton conductivity (10−4 S·cm−1) at 100 °C in the relative humidity range 35–98%. Their luminescence behaviors in the solid state at room temperature have also been investigated. Upon excitation at 384 nm, 1 exhibits three emission peaks centered at 439, 507 and 566 nm. When excited at 364 nm, 2 displays three emission peaks centered at 443, 501 and 553 nm.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2018
·
IF 4.816
Yong-Yu Qi,Qian Gan,Ya-Xian Liu,Ya-Hong Xiong,Zong-Wan Mao,Xue-Yi Le
In the search for more effective anticancer drugs with less toxic side effects, dipeptides were introduced into the Cu(II) complex of 5-methyl-2-(2′-pyridyl)benzimidazole (HPBM). Analytical and spectroscopic techniques were employed to thoroughly characterize complexes [Cu(Gly-gly)(HPBM)(H 2 O)]ClO 4 ·0.5H 2 O ( 1 ) and [Cu(Gly- L -leu)(HPBM)(H 2 O)]ClO 4 ( 2 ) (where Gly-gly = Glycyl-glycine anion, Gly- L -leu = Glycyl- l -leucine anion). The solution stability studies performed by ultraviolet–visible (UV–Vis) spectroscopy confirmed the stability of the complexes in the buffer solutions. The DNA binding affinity was evaluated using multi-spectroscopy, viscosity measurement and molecular docking methods and further quantified by K b and K app values, revealing an intercalative mode. Moreover, gel electrophoresis analysis revealed that the complexes could damage CT DNA through a hydroxyl radical pathway in the presence of ascorbic acid . All the complexes displayed favorable antimicrobial and cytotoxic activities toward the tested microorganisms ( Bacillus subtilis , Staphylococcus aureus , Escherichia coli and Pseudomonas aeruginosa ) and cancer cells (A549, HeLa and PC-3). Most importantly, the possible anticancer mechanism of the complexes was explored by determining the cells morphological changes, intracellular reactive oxygen species (ROS) levels, location in mitochondria, mitochondrial membrane potentials and the expression of Bcl-2 family proteins. The results showed that the complexes could induce apoptosis in HeLa cells through an ROS-mediated mitochondrial dysfunction pathway, which was accompanied by the regulation of Bcl-2 family proteins.
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Materials Research Express
·
2019
·Vol. 6
·期 9
·095315
·
IF 1.449
Huining Zhang,Qing Chang,Jianping Han,Shiming Gao,Zhiguo Wu,Jiawei Hu,Yahong Yang,Zhiqiang Wei,Dengqi Zhang,Zhangpu Peng
In this work, two novel macroporous hydrogel beads (PVA/GO–N and PVA/CS) were prepared to remove Cu2+ and Pb2+ ions in the solution. The maximum Cu2+ sorption capacities on PVA/GO–N and PVA/CS beads were 96.22 and 74.66 mg g−1, while the counterpart sorption capacities of Pb(II) were 278.16 and 144.53 mg g−1, respectively. Isotherm, kinetics and XPS analysis investigation indicated that the sorption processes were controlled by multiple mechanisms. The Cu(II) and Pb(II) removal rates were influenced by the changes of pH, initial dosage, ionic strength, chelator and co-existed ions. The packed-bed sorption column experiments were also carried out to investigate the operating parameters and the potential of the two adsorbents in large scale adsorption systems in practical use. The kinetic model, Thomas equation, was applied to predict dynamic behavior of the fixed bed column for a successful design of a sorption column.
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