ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Tingting Yu,Lei Tao,Zhiyi Liu,Xuge Zhang,Tao Gan,Wensheng Yan,Lirong Zheng,Ge Meng,Wei Chen,Shoujie Liu,Chenliang Ye,Jian Zhang
Unique active sites make single-atom (SA) catalysts promising to overcome obstacles in homogeneous catalysis but challenging due to their fixed coordination environment. Click chemistry is restricted by the low activity of more available Cu(II) catalysts without reducing agents. Herein, we develop efficient, O-coordinated SA Cu(II) directly catalyzed click chemistry. As revealed by theoretical calculations of the superior coordination structure to promote the click reaction, an organic molecule-assisted strategy is applied to prepare the corresponding SA Cu catalysts with respective O and N coordination. Although they both belong to Cu(II) centers, the O-coordinated one exhibits a 5-fold higher activity than the other and even much better activity than traditional homogeneous and heterogeneous Cu(II) catalysts. Control experiments further proved that the O-coordinated SA Cu(II) catalyst tends to be reduced by alkyne into Cu acetylide rather than the N-coordinated catalyst and thus facilitates click chemistry.
研究领域:
化学
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催化
·
材料科学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2018
·
IF 0
Fuhai Li,Dairong Hu,Yahui Yuan,Binbin Luo,Yibing Song,Songtao Xiao,Guanghui Chen,Yiwen Fang,Fushen Lu
To mimic biological enzyme in catalysis, metal-imidazole-salen complexes were proposed (via DFT calculation) and synthesized in situ within the cavities of Y zeolite. Among the synthesized zeozymes, the Cu-salenIIY exhibited a prominent catalytic efficiency for the selective oxidation of benzyl alcohol. Specifically, the activity and selectivity of the encapsulated catalyst were comparable to those of the free Cu-salenII complex in solution. Furthermore, the high activity and selectivity were preserved during the repeated cycles. The similarity in the initial activity implies that the Cu-salenII complex just resides in the cavity of the zeolite Y, and its intrinsic properties responsible for the catalytic activity keep intact after encapsulation. The confinement of zeolite nanocavities effectively inhibited the dimerization or aggregation of the Cu-salenII complex and prevented the active species from escaping into reaction solution, thus resulting in a remarkably improved in the catalytic reusability and durability.
研究领域:
催化
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材料科学
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化学工程
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无机化学
✓ 已验证
产品关联
DOI
JOURNAL OF POROUS MATERIALS
·
2020
·Vol. 28
·期 1
·299-310
·
IF 2.183
Ma Zixuan,Li Fang,Jia Aizhong,Zhang Xiao,Wang Yanji
The highly efficient adsorbents with fast adsorption rate, high adsorption capacity and selectivity as well as good reusability were successfully synthesized through fabricating 3D spherical-chain porous silica material and grafting modification with ethylenediaminetetraacetic acid (EDTA) for the selective removal Cu(II) from wastewater. The obtained adsorbents were characterized by XRD, FT-IR, SEM, TEM, XPS, N 2 adsorption–desorption and back titration. The results indicate that the 3D framework structure is adjustable in a certain range by varying the parameters of the synthesis system. And the adsorption performance of the materials was investigated under different conditions such as pH, contact time and initial metal ions concentration. Under the experiment conditions, the synthesized adsorbent is efficient in removing Cu(II) and the adsorption equilibrium could be achieved within only 5 min, and the kinetic data are well fitted by pseudo-second-order and Langmuir isotherm models. The prepared adsorbents display good selective adsorption of Cu(II) and can be feasibly regenerated without evident decrease even after five recycles. Basing on the obtained results, the plausible adsorption mechanism was proposed and analyzed.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2017
·
IF 3.671
Yuvaraja Gutha,Yaping Zhang,Weijiang Zhang,Xu Jiao
Metal ions cause a serious public health problem. It is a great challenge to find an effective and efficient adsorbent to remove heavy metals from wastewater. Chitosan-based adsorbents are potential and effective for heavy metal ion removal. Hence a novel m-ECCSB was synthesized, characterized and utilized as an adsorbent for the removal of Cu(II) ions from aqueous solution. Various factors affecting the uptake behavior such as pH, adsorbent dosage, contact time, initial concentration of Cu(II) and temperature effect were investigated. Maximum adsorption capability (123.10 mg/g) was obtained at pH = 6, adsorbent dose of = 250 mg, rotational speed = 200 rpm, contact time = 60 min, and temperature of 323 K. The result of the kinetic study shows that the adsorption of Cu(II) could be described by the pseudo-second-order equation. Equilibrium data were analysed with the Langmuir, Freundlich and Dubinin-Radushkevich isotherms and Langmuir model was found to provide the best fit of the experimental data. The thermodynamic parameters showed that the adsorption of Cu(II) onto m-ECCSB was spontaneous (ΔG° = −8.990, −10.00 and −10.593 kJ/mol), endothermic (ΔH° = 15.674, 15.478 and 15.699 kJ/mol) and ΔS° (0.0814 J/mol K) suggests an increased randomness at the solid/solution interface under the studied conditions.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
RSC Advances
·
2022
·Vol. 12
·期 48
·31186-31191
·
IF 4.036
Dandan Jiang,Minghao Zheng,Xiaoyang Yan,Bin Huang,Hui Huang,Tianhao Gong,Kunming Liu,Jinbiao Liu
Herein, we report a highly selective fluorescent probe for the detection of Cu(II). The detection mechanism relies on the Cu(II)-catalyzed oxidative hydroxylation of 2-(aminocarbonyl)phenylboronic acid into salicylamide, thus recovering the excited-state intramolecular proton transfer (ESIPT) effect and inducing more than 35-fold fluorescence enhancement. The simple structure and readily available fluorescent probe give a novel method for quantitatively detecting Cu(II) in the linear range of 0–22 μM, with a limit of detection down to 68 nM, and exhibiting high selectivity for Cu(II) over 16 other metal ions.
研究领域:
分析化学
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材料科学
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光谱学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2019
·
IF 3.834
Zhixing Xiao,Lijuan Zhang,Long Wu,Dan Chen
In this study, a novel adsorbent was synthesized through the entrapment of KMnO 4 modified biochar (MB) in poly(vinyl alcohol)/sodium alginate hydrogel bead (PSMB) and then tested to determine its capacity for removal of Cu(II) from aqueous solutions. The maximum Cu(II) adsorption capacity estimated with Langmuir isotherm modeling was 87.07 mg/g of PSMB, which was higher than that of previously reported adsorbents. PSMB had a good selectivity towards Cu(II) as well as high anti-interference ability. The main species for Cu(II) adsorption likely were the inner-sphere Cu-O complexes, as indicated by the results of spectral analyses. The PSMB was easily collected and exhibited a minimal loss of adsorption capacity after 10 adsorption/regeneration cycles. The effective removal of Cu(II) from environmental water samples with relative low treatment cost indicated a possibility for practical application.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2021
·
IF 6.953
Ping Sun,Wei Zhang,Binze Zou,Lincheng Zhou,Zhengfang Ye,Quanlin Zhao
Attapulgite (ATP) has a unique porous layered chain structure and is an excellent environment-friendly decolorizer. However, its high viscosity makes it difficult to separate. First, it was combined with magnetic Fe 3 O 4 nanoparticles to obtain Fe 3 O 4 -ATP that is easy to recycle and reuse. Then, Fe 3 O 4 -ATP nanoparticles were embedded in chitosan (CS) gel beads, and glutaraldehyde was used for cross-linking and curing. Lastly, ethylenediaminetetraacetic acid (EDTA) was successfully connected to Fe 3 O 4 -ATP/CS gel beads through amidation reaction, which further increased the capability of the adsorbent to adsorb heavy metal ions. The prepared magnetic composite adsorbent is a sphere with a rough surface and porous structure. The maximum adsorption capacity of the prepared Fe 3 O 4 -ATP/EDTA/CS adsorbent for Pb(II), Cu(II), and Ni(II) is 368.32, 267.94, and 220.31 mg g −1 , respectively. After 5 times of repeated use, Fe 3 O 4 -ATP/EDTA/CS still showed good adsorption capacity for Cu(II), Pb(II), and Ni(II). Fe 3 O 4 -ATP/EDTA/CS has a large adsorption capacity for heavy metal ions, a wide pH applicability, good reuse, and rapid magnetic separation. In addition, Cu(II) loaded Fe 3 O 4 -ATP/EDTA/CS also showed good catalytic degradation performance for bisphenol A. This study prepared a new type of adsorbent with good adsorption performance and provided a promising method for the treatment of wastewater.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
IONICS
·
2021
·Vol. 27
·期 10
·4439-4448
·
IF 2.817
Huang Xiangjin,Li Jianwen,Xie Chunsheng,Zhang Huasheng,Wei Shoulian,Lai Wenfeng,Xian Shaoling,Huang Sicong
Herein, a nanocomposite comprising polyvinyl pyrrolidone (PVP) and cobalt(II) hydroxide (Co(OH) 2 ) nanoparticles (PVP–Co(OH) 2 ) was synthesized via a hydrothermal method and used for detection of Cu(II) ions. Using PVP grafted nanosized Co(OH) 2 as a surfactant could decrease the aggregation and reduce the particle size. The conducted morphology investigations showed that PVP–Co(OH) 2 nanocomposite was composed of small spherical particles with a diameter of 40–80 nm that could accelerate mass diffusion and favor the deposition-stripping process of Cu(II) ions. High catalytic activity of Co(OH) 2 and good affinity of PVP to Cu(II) ions synergistically enhances sensing performance of the PVP–Co(OH) 2 nanocomposite-modified electrode than Co(OH) 2 - and PVP-modified electrodes. A linear response was obtained for Cu(II) ion concentration over a range of 1.0–90.0 μg/L, with a detection limit of 0.26 μg/L (S/N = 3). The proposed electrode exhibited good performance in terms of selectivity, stability, and reproducibility. It was also employed to detect Cu(II) ions in water and food samples, and the results were in good agreement with those obtained by graphite furnace atomic absorption spectrometry.
研究领域:
分析化学
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2016
·
IF 3.698
Ying Han,Zhong-lin Chen,Ji-min Shen,Ji-he Wang,Wei-wei Li,Jun Li,Bin-yuan Wang,Li-na Tong
The role of Cu(II) in the reduction of N -nitrosodimethylamine (NDMA) with zero-valent metals was investigated by determining the effects of Cu(II) on the removal, kinetics, products, and mechanism. NDMA removal was enhanced, and all reactions followed a pseudo-first-order kinetic model except for the Fe and Fe/0.1 mM Cu(II) systems. The iron mass-normalized pseudo-first-order rate constants ( k MFe ) increased with the Cu(II) concentration. The zinc mass-normalized pseudo-first-order rate constants ( k MZn ) were identical to those with the Cu(II) concentrations from 0.1 mM to 1.0 mM and were higher with 2.0 mM Cu(II). The types of products detected were unchanged. Some unknown products were also found. NDMA was reduced to 1,1-dimethylhydrazine (unsymmetrical dimethylhydrazine , UDMH). Then, UDMH was reduced into dimethylamine (DMA) by the Fe/Cu(II) and Zn/Cu(II) systems. Catalytic hydrogenation was proposed as the reduction mechanism. Several copper species, such as Cu(OH) 2 in the Fe/Cu(II) system and Cu 2 O and Cu(OH) 2 in the Zn/Cu(II) system enhanced NDMA reduction. Differences between the Fe/Cu(II) and Zn/Cu(II) systems were caused by the reduction potentials and surface conditions of the different metals and the copper species in the various systems.
研究领域:
环境化学
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水处理
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催化
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
POLYMER
·
2018
·
IF 3.483
Hongde Lei,Lu Liu,Lukuan Huang,Weixing Li,Weihong Xing
In this study, we fabricated a novel anti-fouling poly(vinylidene fluoride) (PVDF) membrane using a novel amphiphilic copolymer of PVDF grafted with tetrahydrofurfuryl methacrylate (PVDF-g-THFMA). This copolymer was synthesized via photoinduced Cu(II)-mediated reversible deactivation radical polymerization . The amphiphilic copolymer was characterized by 1 H nuclear magnetic resonance and Fourier transform infrared spectroscopy . The morphology of the copolymer was examined using scanning electron microscopy. The permeability and hydrophilicity of the membranes were evaluated on the basis of their pure water flux and dynamic contact angles, respectively. The anti-fouling property of the membranes was evaluated by carrying out filtration using a bovine serum albumin (BSA) solution. The PVDF-g-THFMA copolymer membranes showed a pure flux of up to 293.9 L m −2 h −1 bar −1 and a molecular weight cut off of 39.5 kDa. After the filtration of the BSA solution, the PVDF-g-THFMA copolymer membrane was washed with deionized water and the recovery ratio of the pure water flux reached a value of 89.1%. The modified membrane showed good filtration performance and anti-fouling property.
研究领域:
材料科学
·
环境工程
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nanoscience and Nanotechnology Letters
·
2019
·Vol. 11
·期 10
·1366-1374
·
IF 0
Ding Zhexu,Yang Haiyu,Du Min,Ruan Xiaofang,Luo Jun,Chen Sha,Li Ding
Nowadays, extensive use of copper in electric industries has severely contaminated aquatic environments. To address this issue, combining fungal biomass with nanomaterials is considered as an efficient way for adsorbing heavy metals from wastewater. In this work, a novel composite material
"Fungal mycelium coupled with Carbon nanotubes" (FM-CNTs) was synthesized and used for adsorption of Cu(II) ions in aqueous solution. To begin with, potassium permanganate and concentrated nitric acid were used as strong oxidants to modify the surface of CNTs, creating additional carboxyl
groups for coupling with amine groups from the surface of FM. Next, various characterization approaches such as SEM-EDX, FT-IR, XPS and TGA, were used to investigate the interaction between FM-CNTs and Cu(II) ions. Characterization results showed that the surface of FM-CNTs were significantly
changed after absorbing Cu(II) ions. Further, the effect of pH on adsorption capacity of FM-CNTs for Cu(II) was explored, showing that FM-CNTs had the best adsorption performance at pH of 5. Finally, Langmuir-Freundlich isothermal models were performed to analyze the adsorption behavior of
FM-CNTs for Cu(II). The experimental data from the adsorption of Cu(II) by FM-CNTs were best fitted to the Langmuir model, and the maximum adsorption amount of the FMCNTs for Cu(II) was found to be 342.22 mg/g. More importantly, FM-CNTs showed better adsorption capacity than fungal mycelium
alone. Overall, FM-CNTs exhibited excellent performance for adsorption of Cu(II) ions, thus greatly broadening its application prospects in copper-contaminated wastewater treatment.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
DOI
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Haorui Wang,Haodan Xu,Wei Cheng,Yinwen Luo,Tao Zhang,Jun Ma
Iodinated contrast media compounds (ICMs) are intensively applied in medical diagnostic radiology and have received wide environmental concerns due to formation potential of iodinated disinfection byproducts. Conventional water/wastewater treatment processes cannot effectively remove ICMs; reducing their total organic iodine concentration is even more difficult. The source control or elimination of ICMs thus becomes necessary. We report here that the refractory ICMs (5 μM) can be efficiently deiodinated by ascorbate/ascorbic acid (AA) (200 μM) coupled with a trace amount of Cu(II) (5 μM) through catalytic reduction but not oxidation, contrary to the conventional concept of AA/Cu(II) coupling, which produces reactive oxygen species. Taking diatrizoate (DTZ, a refractory ICM) as an example, the coupling completely deiodinated DTZ without destroying its molecular structure. High-performance liquid chromatography inductively coupled plasma mass spectrometry analysis revealed that ternary complexes form between Cu(II), ascorbate, and the anilide moiety of DTZ. Cu(II) in the ternary complex works as an efficient electron-transfer shuttle to convey electrons from ascorbate to the target compound, inducing sequential and complete deiodination. Both DTZ and the nonionic ICMs can be effectively deiodinated even in human urine. Thus, AA coupled with trace Cu(II) could be potentially useful for the source elimination of organic iodine of ICMs.
研究领域:
环境科学
·
化学
·
水处理技术
✓ 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）