CHEMOSPHERE
·
2019
·
IF 5.108
Jiajun Long,Longqian Xu,Linghui Zhao,Huaqiang Chu,Yunfeng Mao,Deli Wu
In this study, Cu(0) was synthesized with NaBH 4 as a reducing agent for Cu(II) and used to activate dissolved molecular oxygen (O 2 ) under acidic conditions. The Cu(0) synthesized had much higher activity than the purchased. The roles of Cu was clarified and the formation of reactive oxygen species was discussed through direct detection for the first time. By detecting the valence change of Cu in a CuO system, Bisphenol A (BPA) was found to accelerate the transformation of Cu(II) to Cu(I). Besides, the evidence from electron spin resonance (ESR) studies and scavenging tests revealed the new roles of Cu(0) that Cu(0) could not only convert O 2 to produce ·O 2 − , but also catalyze H 2 O 2 to ·OH. The results from this study offer evidence of new reaction pathways in Cu-activated O 2 systems and deepen understanding of the reaction between Cu species and O 2 .
研究领域:
环境科学
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化学
·
材料科学
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DOI
PubMed
高影响因子
Chem
·
2023
·
IF 23.5
Rongming Cai,Mingzi Sun,Fei Yang,Min Ju,Yanpeng Chen,M. Danny Gu,Bolong Huang,Shihe Yang
Summary By leveraging a Cu(OH)F precursor, we construct a disk-like Cu(I)/Cu(0) interface model (P-Cu x /Cu 2 OF) composed of F-stabilized Cu(I) shell and Cu(0) core by one-step pulsed potential conversion. The interfacial region is shown to facilitate ethanol formation, guaranteeing a high FE(C 2+ ) of up to 80.2%. Tuning the Cu(I)/Cu(0) ratio enhances the ethanol yield by 18.5-fold over pure P-Cu, with the corresponding partial current density (j ethanol ) reaching up to 128 mA/cm 2 . This is enabled by a 3.6-fold boost in selectivity for the ethanol product (35.4%) and an overall 7.8-fold boost in activity ( j C 2 + up to 288 mA/cm 2 ). The interactions between P-Cu and Cu 2 OF upshift the d-band center of Cu sites on the interface region, which is critical to asymmetrical C-C coupling to form OCCOH∗, concurrent with a lowered energy barrier for ethanol formation. On the other hand, the ethylene-forming symmetrical C-C coupling occurs primarily on P-Cu away from the Cu(I)/Cu(0) interface.
研究领域:
材料科学
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电化学
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催化
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可再生能源
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DOI
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
·
2021
·
IF 3.975
Yingdong Duan,Qizheng Li,Biyun Peng,Shaobo Tan,Zhicheng Zhang
In the present work, diverse vinyl monomers were successfully grafted onto poly(vinylidene fluoride-hexafluoropropylene) P(VDF-HFP) via direct activation of C F bonds using Cu(0)/4,4′-dimethyl-2,2′-bipyridyl (DMDP) as catalyst under mild conditions. The structure of the graft copolymer was carefully characterized, and the initiating site was confirmed at the same time. Moreover, the kinetic results indicated the controlled behavior of the graft polymerization, and the composition of the graft copolymer can be regulated by changing the reaction conditions. This work may provide a facile strategy to endow P(VDF-HFP) copolymer with new functions via directly activating C F bonds.
研究领域:
材料科学
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高分子化学
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产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 87
·70758-70765
·
IF 3.84
Leli Wang,Ying Wu,Yongjun Men,Jianan Shen,Zhengping Liu
Single electron transfer living radical polymerization (SET-LRP) was employed to prepare thermal-sensitive starch graft poly(N-isopropylacrylamide) (Starch-g-PNIPAM) with soluble Starch-Br as macro-initiator at molecular level. And Starch-g-PNIAPM with improved graft ratio and controlled length of graft chains were obtained. The effects of molar ratio of monomer to initiator and temperature on polymerization were investigated. The thermal responsibilities investigated by 1H NMR and UV showed that the LCST ranged from 31.5 °C to 23 °C with the increase of the length of PNIPAM chains and the concentrations of copolymers. Starch-g-PNIPAM hydrogels were gained when adding N,N′-methylenebisacrylamide as crosslinking agent and the swelling and deswelling behaviors were also investigated. The obtained hydrogels possess a high equilibrium swelling ratio as high as 1826%, and an extremely rapid shrinking rate as fast as losing more than 85% of water in 5 min.
研究领域:
高分子化学
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材料科学
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产品关联
DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 14
·e202300180
·
IF 8.4
Yinjian Zheng,Zhiyuan Wang,Peng Chen,Wenbiao Zhang,Qingsheng Gao
Graphical Roughness-dependence of Cu electrodes is for the first time identified in the electro-reductive coupling of nitro and carbonyl compounds. With increased roughness, the selectivity of nitrones decreases, while that of imines increases, thanks to the feasible control over the reduction of nitroarenes to hydroxylamines or amines on Cu I /Cu 0 interfaces. The electro-reductive coupling of nitro and carbonyl compounds enables a facile, environmentally friendly and energy benign transformation toward value-added nitrones or imines, but the selectivity is still challenging. Here, the surface roughness of Cu electrodes is introduced for the first time as the determinant to switch products from nitrones to imines owing to the controllable reduction of nitroarenes to hydroxylamines or amines on tailored Cu I /Cu 0 interfaces. The roughness-dependent selectivity, that is the decrease of nitrones and the increase of imines with enhanced roughness, is visible in the electro-reductive coupling of nitrobenzene and furfural. Thus, the high selectivity of nitrone (98 %) and imine (80 %) can be achieved on a surface smooth Cu foil and the one electrochemically roughened in the presence of I − , respectively. Such roughness-dependence of nitrone/imine selectivity on Cu electrodes is further verified in a wide substrate scope, highlighting the promise of surface/interfacial engineering for electrochemical synthesis.
研究领域:
电化学
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有机合成
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材料科学
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表面科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
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2013
·Vol. 51
·期 6
·1468-1474
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IF 3.543
Yun-Hai Yu,Xiao-Hui Liu,Di Jia,Bo-Wen Cheng,Fei-Jun Zhang,Hui-Na Li,Peng Chen,Shan Xie
Zn(0)/ppm concentrations of CuBr 2 from 10 to 50 ppm was firstly used to catalyze radical polymerization of acrylonitrile at ambient temperature. The polymerization displayed typical living radical polymerization (LRP) characteristics, as evidenced by pseudo first-order kinetics of polymerization, linear increase of number-average molecular weight, and low polydispersity index (PDI) value. Effects of solvent, copper concentration, and initiator concentration on the polymerization reaction and molecular weight as well as PDI were investigated in detail. EC excelled NMP, DMF, and DMSO in terms of rate of polymerization as well as control of molecular weight and PDI. The increase of the copper concentration from 2.5 to 50 ppm leads to a higher rate of polymerization and a better control over the polymerization reaction. 1 H NMR and GPC analyses as well as chain extension reaction confirmed the very high chain-end functionality of the resultant polymer. © 2013 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2013
研究领域:
高分子化学
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材料科学
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有机合成
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自由基聚合
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DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 14
·8484-8490
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IF 3.108
Hui Xue,Lun Peng,Yishi Dong,Yuqing Zheng,Yafei Luan,Xiang Hu,Gaojian Chen,Hong Chen
In this paper, novel star glycopolymers were synthesized via Cu(0)-mediated radical polymerisation at ambient temperature. The reaction was fast with little star–star coupling. Moreover, star glycopolymers can be obtained without removing oxygen from the polymerisation mixture. The effects of solvent and the ratio of initiator/catalyst/ligand on polymerisation were investigated, and the optimal conditions for the synthesis of star glycopolymer were determined. In addition, the binding ability between synthesised glycopolymers and concanavalin A (ConA) was studied using a turbidity test and quartz crystal microbalance-dissipation (QCM-D). Compared with linear glycopolymers, star glycopolymers showed higher binding ability to specific lectins and the strongest binding was obtained when the molecular weight was medium.
研究领域:
高分子化学
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材料科学
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生物化学
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DOI
高影响因子
JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
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2013
·Vol. 51
·期 7
·1559-1564
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IF 3.543
Xiao-Hui Liu,Yun-Hai Yu,Di Jia,Bo-Wen Cheng,Fei-Jun Zhang,Hui-Na Li,Peng Chen,Shan Xie
Single electron transfer living radical polymerization of methyl methacrylate catalyzed by the in situ prepared Cu(0) at ambient temperature was first examined using various metallic powders, including Zn(0), Ni(0), Mg(0), and Fe(0). Importantly, the polymerization initiated with Ni(0)/EBiB/CuBr 2 /PMDETA system exhibited optimal living/controlled nature and generated polymers with polydispersity index as low as 1.04 for 75.27% conversion and controlled molecular weights close to theoretical ones. A wide of range of Cu(II) salts were also investigated as catalyst sources instead of CuBr 2 . The recycling of Ni(0) was very convenient due to its magnetic property, which enables its extensive application. © 2013 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2013
研究领域:
高分子化学
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材料科学
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催化化学
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有机合成
·
功能材料
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DOI
高影响因子
POLYMER BULLETIN
·
2015
·Vol. 72
·期 10
·2455-2469
·
IF 1.438
Bai Liangjiu,Wang Dongju,Chen Hou,Li Dongxin,Xu Yuanyuan,Yu Lili,Wang Wenxiang
Abstract Peanut shell (PNS) was used to prepare a novel adsorbent to achieve resource recovery of the agricultural residue. The hydroxyl groups of peanut shell were turned into –C(CH 3 ) 2 –Br pendant groups to initiate polymerization of acrylonitrile. Graft copolymer peanut shell/polyacrylonitrile (PNS- g -PAN) was modified by hydroxylamine hydrochloride to transform the cyano groups into amidoxime (AO) groups. The modified copolymer of AO-PNS- g -PAN was used as adsorbent. The maximum adsorption capacity for Hg(II) was 4.45 mmol g −1 . The adsorption process fitted well the Freundlich isotherm model and followed pseudo-second-order model. The modified copolymer demonstrated its potential as an efficient adsorbent to solve the problem of Hg(II) contamination. Graphical abstract The peanut shell (PNS) macroinitiator was obtained by acylation of hydroxyl groups on the cellulose backbone of the peanut shell and initiated by Cu(0)-mediated RDRP of acrylonitrile. PNS- g -PAN was modified by NH 2 OH·HCl and used to remove heavy metal ions. The maximum adsorption capacity of Hg(II) was 4.45 mmol g −1 .
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
MACROMOLECULES
·
2021
·
IF 5.985
Sikai Chen,Ze-Lian Zhang,Fei Song,Xiu-Li Wang,Yu-Zhong Wang
Facing the limitation of weak compatibility on the use of cellulose nanofiber (CNF) as a reinforcement in polymer matrix nanocomposites, this work developed an alternative approach to fabricating a series of one-component CNF-reinforced nanocomposites by grafting polyacrylates from CNF via surface-initiated Cu(0)-mediated reversible deactivation radical polymerizations. An initiator group was initially introduced onto the surface of CNF through one-step esterification. Then, graft polymerization of methyl acrylate and n-butyl acrylate was carried out to obtain polyacrylate-grafted CNF. The graft polymerization exhibited several advantages, including simplicity, rapidity, and effectivity. A high graft ratio (up to 3000%) was obtained at room temperature after 3 h. The graft ratio was controlled by regulating the monomer concentration and reaction time. Characterizations confirmed that the chemical, morphological, and crystalline structure of CNF was maintained after surface modification and grafting. The uniform morphology and moderated transparency of solvent-casting polyacrylate-grafted CNF films proved the superior homogeneity of these nanocomposites. Tensile experiments revealed that poly(methyl acrylate)-grafted CNF nanocomposites had remarkable mechanical properties (tensile strength = 13.6–25.3 MPa; break elongation = 48.8–179.9%), contributing to an outstanding dispersity. By alternating the graft ratio, the mechanical behavior of the nanocomposite could transition from tough to ductile. This grafting approach has been proven to be a powerful tool for the design of CNF-reinforced nanocomposites for various purposes.
研究领域:
材料科学
·
高分子化学
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DOI
高影响因子
BIOMACROMOLECULES
·
2018
·
IF 5.738
Donghao Wang,Wenyi Ding,Kaiyue Zhou,Shutong Guo,Qiang Zhang,David M. Haddleton
Immobilization of enzyme could offer the biocatalyst with increased stability and important recoverability, which plays a vital role in the enzyme’s industrial applications. In this study, we present a new strategy to build an intelligent enzyme carrier by coating titania nanoparticles with thermoresponsive epoxy-functionalized polymers. Zero-valent copper-mediated living radical polymerization (Cu(0)-LRP) was utilized herein to copolymerize N-isopropylacrylamide (NIPAM) and glycidyl acrylate (GA) directly from an unprotected dopamine-functionalized initiator to obtain an epoxy-containing polymer with terminal anchor for the “grafting to” or “one-pot” modification of titania nanoparticles. A rhodamine B-labeled laccase has been subsequently used as a model enzyme for successful immobilization to yield an intelligent titania/laccase hybrid bifunctional catalyst. The immobilized laccase has shown excellent thermal stability under ambient or even relatively high temperature above the lower critical solution temperature (LCST) at which temperature the hybrid particles could be facilely recovered for reuse. The enzyme activity could be maintained during the repeated use after recovery and enzymatic degradation of bisphenol A was proven to be efficient. The photocatalytic ability of titania was also investigated by fast degradation of rhodamine B under the excitation of simulated sunlight. Therefore, this study has provided a facile strategy for the immobilization of metal oxide catalysts with enzymes, which constructs a novel bifunctional catalyst that will be promising for the “one-pot” degradation of different organic pollutants.
研究领域:
生物化学
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材料科学
·
环境科学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Peng Xu,Jiaqi Feng,Na Li,Jiafan Yao,Guangchao Li,Baolin Hou
Zero-valent copper (Cu(0))-activated peroxodisulfate (PDS) generates reactive oxygen species (ROS) that effectively degrade azo dyes, but its application is limited by low Cu(I) conversion and narrow pH range. To overcome these barriers, this study introduced hydroxylamine (HA) to the Cu(0)/PDS system, boosting its oxidative capacity by accelerating the Cu(I)/Cu(II) redox cycle. Under the optimal conditions, the Cu(0)/PDS/HA system achieved a 78.5 % improvement in the degradation efficiency of orange II (AO7) within 10 min. UV-Vis spectroscopy, electron spin resonance (ESR) analysis, and scavenging experiments confirmed SO 4 •- and • OH as the primary reactive species in the Cu(0)/PDS/HA system, with minimal Cu(III) formation. A Systematic investigation of operational parameters (initial pH, Cu(0) dosage, HA concentration, and PDS concentration) and water matrix components (Cl - , NO 3 - , SO 4 2- , HCO 3 - , and humic acid) revealed their impact on AO7 removal. Furthermore, experiments in real water samples (tap, lake, and river water) validated the practicality of the Cu(0)/PDS/HA system, which was also demonstrated to effectively degrade other common pollutants. In conclusion, the present study provided an efficient strategy to bolster the oxidizing capacity of Cu(0)/PDS system, broadening its application potential for treating refractory organic pollutants.
研究领域:
环境科学
·
化学工程
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产品关联
DOI
高影响因子