GREEN CHEMISTRY
·
2021
·Vol. 24
·期 1
·384-393
·
IF 10.182
Qi Zhang,Shouxin Liu,Xia Tian,Yidong Liu,Shiming Fan,Baibiao Huang,Andrew Whiting
A highly selective, green and sustainable chlorination of aliphatic C–H bonds is reported using MCln under the co-catalysis of visible light and nano-Cu@CuCl, which was synthesised via a one-step, hydrothermal strategy using copper(II) sulfate and D-glucose as the reducing agent in a KCl solution. A novel cascade method of producing Cl2 occurs in situ chlorinating C(sp3)–Hs, achieved through nano-Cu@CuCl catalysis using inorganic chloride MCln as a chlorine source under visible light and without the need for a strong oxidant. The reaction was applied to the chlorination of different alkylarene α-Hs and cyclic hydrocarbons C–HS and was developed for use in a photocatalytic serial reactor system which accomplished the chlorination of toluene α-Hs to give 92% conversion, 90% yield and 98% selectivity. Electron spin resonance (ESR) studies of DMPO-Cl. revealed that the reaction mechanism belonged to a free radical process.
研究领域:
有机化学
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绿色化学
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材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 59
·54623-54635
·
IF 3.289
Jing Wang,Chao Liu,Ijaz Hussain,Cheng Li,Jiansheng Li,Xiuyun Sun,Jinyou Shen,Weiqing Han,Lianjun Wang
A series of iron–copper bimetallic nanoparticles supported on hollow mesoporous silica spheres with different Fe/Cu ratios were prepared using a simple post-impregnation and sodium borohydride reduction strategy. Different Fe/Cu ratios were obtained by addition of various amounts of ferric and copper salts. The catalysts were characterized by XRD, XPS, nitrogen physisorption, SEM and TEM. To explore the difference of catalytic reactivity among the various FeCu/HMS composites, Fenton-like catalytic oxidation of orange II was chosen as the model catalysis reaction. The catalytic results showed that the catalytic activity depended highly upon the Fe/Cu ratio. Particularly, 1/3 (2Fe6Cu/HMS) is the optimum Fe/Cu mass ratio to achieve the best catalytic activity. Based on the results of detection of ˙OH radicals and cyclic voltammograms, the important origin of the synergetic effect in 2Fe6Cu/HMS is considered as the combination of iron and copper species, which can accelerate the interfacial electron transfer in redox cycles of Fe3+/Fe2+ and Cu2+/Cu+ pairs, followed by the increase in the ˙OH radical generation. The 2Fe6Cu/HMS also possesses less pH dependence and maintains its high activity even under alkaline conditions. The optimal parameters in the degradation of 100 mg L−1 orange II are 27.4 mM of H2O2 with 1.0 g L−1 of catalyst, performed at a pH of 7.0 and 30 degree celsius. It is worth noting that 2Fe6Cu/HMS also possesses potential to treat a high concentration of dye pollutants. 77.7% of orange II was removed when conducted at 1000 mg L−1 initial dye concentration. The stability and recoverability of the composite catalyst were assessed it exhibited a good performance after 5 consecutive runs. The as-synthesized composite catalyst proved to be an attractive alternative for dye wastewater treatment applications.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·737-749
·
IF 6.119
Zhicheng Xu,Yuran Li,Yuting Lin,Bin Wang,Panting Gao,Tingyu Zhu
The reduction of NO by CO was proposed to be applied for regeneration gas to remove NOx from industrial flue gas with activated carbon purification technology. To improve the activity and sulfur resistance for the reduction of NO by CO in regeneration gas, Cu and Fe modifications on activated carbon were investigated. And various samples were characterized by XRD, XPS, TPD, H2-TPR, in situ DRIFTS and DFT calculations to explain the reaction mechanism and poisoning mechanism. The synergistic effects of oxygen-containing functional groups and metal sites show that –COOH acts as an anchor site for metals and that C–O–C acts as a protective site for Fe3+ under a SO2 atmosphere. Cu2+ sites have a high activity at low temperatures due to the large amount of adsorbed NO and the intermediate NOx− participating in the reaction with the NOx− pathway. Fe3+ sites have a high activity at high temperatures due to the high N–O dissociation activity with the *N pathway and –NCO pathway. DFT calculations proved that the binding Cu2+ and Fe3+ sites have higher activity than free Cu2+ and Fe3+ sites. A high content of SO2 exhibits various poisoning effects, mainly including the sulfation of metal sites, deposition of S, and consumption of CO. AC-Fe-H exhibits excellent resistance and stability against SO2 and H2O due to less S deposition caused by consumption through the S–CO reaction, slight sulfation caused by the protective effect of Fe2+ and C–O–C on Fe3+ sites and better hydrophobicity.
研究领域:
环境科学
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化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Ruxia Song,Shihong Zhang,Yi He,Hongjie Li,Yi Fan,Teng He,Yihan Zhang,Yuxin Xiang,Huili Zhang
Ni-Cu/H-MWCNTs composite coatings with outstanding corrosion resistance and high wear resistance were prepared by the pulse electrodeposition technology. The micro-surface morphology and corrosion behavior of the coatings were represented by high-resolution field emission scanning electron microscopy , potential polarization curve, electrochemical impedance spectroscopy and scanning electrochemical microscope. The chemical composition and crystal structure of the coatings were characterized by energy dispersive spectrum, X-ray photoelectron spectroscopy and X-ray diffraction. The mechanical properties are studied by digital microhardness tester and multifunctional material surface testing machine. We found that the successful doping of H-MWCNTs changed the micro-structure and morphology of the Ni-Cu-based coating, making the coating smoother and denser. Furthermore, the average crystallite size of the Ni-Cu/H-MWCNTs (0.5 g/l) composite coating is 13.28 nm. The microhardness and average friction coefficient of the composite coating (0.5 g/l) are 587.04 Hv and 0.178, respectively. It was also found that the composite coating (0.5 g/l) has the best anti-corrosion performance, which is 3.2 times that of the pristine Ni-Cu-based coating. Through SECM diagrams, the composite coating (0.5 g/l) has excellent pitting resistance in 3.5 wt % NaCl solution.
研究领域:
材料科学
·
电化学
·
表面工程
✓ 已验证
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 44
·26142-26150
·
IF 3.119
Binyu Xu,Samuthirarajan Senthilkumar,Wei Zhong,Zhongquan Shen,Chunxin Lu,Xiaoming Liu
In this work, core–shell Fe3O4@Cu2O and Fe3O4@Cu2O–Cu nanomaterials for aerobic oxidation of benzylic alcohols are reported with 2,2,6,6-tetramethylpiperidine-N-oxyl (TEMPO) and N-methylimidazole (NMI) as the co-catalysts. To anchor Cu2O nanoparticles around the magnetic particles under solvothermal conditions, the magnetic material Fe3O4 was modified by grafting a layer of L-lysine (L-Lys) to introduce –NH2 groups at the surface of the magnetic particles. With amine groups as the anchor, Cu(NO3)2 was used to co-precipitate the desired Cu2O by using ethylene glycol as the reducing agent. Prolonging the reaction time would lead to over-reduced forms of the magnetic materials in the presence of copper, Fe3O4@Cu2O–Cu. The nanomaterials and its precursors were fully characterized by a variety of spectroscopic techniques. In combination with both TEMPO and NMI, these materials showed excellent catalytic activities in aerobic oxidation of benzylic alcohols under ambient conditions. For most of the benzylic alcohols, the conversion into aldehydes was nearly quantitative with aldehydes as the sole product. The materials were recyclable and robust. Up to 7 repeat runs, its activity dropped less than 10%. The over-reduced materials, Fe3O4@Cu2O–Cu, exhibited slightly better performance in durability. The magnetic properties allowed easy separation after reaction by simply applying an external magnet.
研究领域:
材料科学
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催化
·
化学工程
·
纳米技术
✓ 已验证
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Yong Sun,Caixia Xiong,Quanchang Liu,Jiaren Zhang,Xing Tang,Xianhai Zeng,Shijie Liu,Lu Lin
Compared to biomass-derived 5-hydroxymethylfurfural (HMF), 5-formyloxymethylfurfural (FMF) is highly potential as feedstock to produce 2, 5-dimethylfuran (DMF) due to its properties of higher stability and enhanced hydrophobicity. Herein, catalytic conversion of FMF to DMF over Ni–Cu bimetallic catalyst with formic acid (FA) as hydrogen donor was investigated. A favorable DMF yield of 71.0% was obtained by catalyst 36Ni-12Cu/SBA-15. The conversion of FMF to DMF was controlled by surface reaction on the catalyst. In addition, catalytic mechanism investigation showed that the excellent catalytic performance and recyclability of catalyst were attributed to the formation of Cu–Ni alloy and its synergistic role. The incorporation of Cu and Ni substantially improved the selectivity of hydrogenolysis toward C–O ester bond. Meanwhile, FMF exhibited a better advantage to substitute HMF for producing DMF over Ni–Cu bimetallic catalyst with formic acid as a hydrogen donor.
研究领域:
化学工程
·
生物质能
·
催化科学
✓ 已验证
DOI
高影响因子
FOOD CHEMISTRY
·
2022
·
IF 9.231
Haiyang Wang,Lin Cai,Yuwei Wang,Chang Liu,Guozhen Fang,Shuo Wang
A molecularly imprinted electrochemical sensor (MIES) modified with Cu-MOF and Ti 3 C 2 Tx was successfully prepared for the detection of hygromycin B in food. According to the pH sensitive property of reversible borate ester bonds, a molecularly imprinted polymers (MIP) were constructed on the modified gold electrode (GE) surface by electropolymerization to realize the controllable elution and adsorption of template molecules. Cu-MOF with large specific surface area and Ti 3 C 2 Tx with excellent electrical conductivity cooperate to improve the overall analytical performance of MIES. The morphology and electrochemical performance of the sensor were evaluated. Under the optimal experimental conditions, the method showed superior selectivity to hygromycin B with a linear range of 5 × 10 −9 –5 × 10 −6 M and a detection limit of 1.92 × 10 −9 M (S/N = 3). The detection results of this method are in good agreement with HPLC-MS/MS, which proves that the method has reliable practicability and accuracy.
研究领域:
食品科学
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分析化学
·
生物传感技术
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Yanru Zhu,Jian Zhang,Xiaodan Ma,Zhe An,Shaowei Guo,Xin Shu,Hongyan Song,Xu Xiang,Jing He
Complexity of chemical linkages (C-C/C-H/C-O, C=C/C=O, or C-O-H/C-O-C) in biomass-derived molecules makes the selective activation of targeted bonds much more challenging, expecting well-defined catalysts and definite catalytically-active sites. This work demonstrates an effective gradient reduction strategy to control the definite structure of catalytically-active sites, affording defects-rich nano-twin Cu particles. This strategy just involves the reduction (calcination under H 2 ) of Cu II -containing layered double hydroxides (LDHs) simply with controlling the reduction gradient (interval time) of Cu II species in two chemical micro-environments (Cu II -O-Cu II and Cu II -O-M II/III/IV (M ≠ Cu)) in the brucite-like layer of LDHs. The nano-twin Cu particles efficiently promote the target activation of C-O and C=C in the conversion of furfural to cyclopentanone (CPO). With ~100% furfural conversion, the defects-rich nano-twin Cu particles afford a CPO selectivity of 92%, 50% higher than regular spherical Cu particles. The multi-stepped defect sites, originating from the planar defects, play a decisive role in promoting the CPO selectivity by facilitating the hydro-deoxygenation to C-O of 4-hydroxycyclopentenone (HCP) and hydrogenation to C=C of HCP or cyclopentenone.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Mingran Li,Xia Qin,Jiaxin Cui,Rui Guo,Chengrui Guo,Ziyuan Wang,Tinghui Li
In this study Cu-Fe bimetallic aerogel-like carbon based on sodium alginate (SA) was prepared as catalytic particle electrode by freeze-drying and carbonization process. The characterization indicates that Cu and Fe were loaded on the surface and inside SA-based biomass carbon (SAC) in the form of a zero-valent copper-iron alloy to form a Cu-Fe/Sodium alginate Carbon (Cu-Fe/SAC) particle electrode. After using a three-dimensional Electro-Fenton (3D-EF) system with the prepared particle electrode, the optimal experimental operating parameters for removal of fulvic acid (FA) were obtained as follows: voltage 2.5 V, pH 5.4, and catalyst dosage 4 g/L. A removal efficiency from 82.9% to 74.4% for FA was achieved in a wide pH range of 3–7. Comparison experimental results indicate that the 3D-EF system with bimetallic Cu-Fe/SAC as the catalytic particle electrode (CPE) has higher FA degradation rate and mineralization efficiency than two-dimensional Electro-Fenton (2D-EF) system, even higher than the 3D-EF system with Cu/SAC or Fe/SAC. Hydroxyl radicals (·OH) trapping experiments showed that the main contribution to FA degradation and mineralization in the 3D-EF system would be the ·OH radical produced by a heterogeneous Fenton-like reaction. The comparison and trapping experiment results indicate that the possible mechanism of the 3D-EF with Cu-Fe/SAC as CPE for FA degradation may involve adsorption, anode oxidation, heterogeneous and homogeneous Fenton-like reactions.
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2020
·
IF 3.104
Di Deng,Shujun Deng,Dandan He,Zhiheng Wang,Zhipeng Chen,Yi Ji,Guoping Yan,Guangjin Hou,Licheng Liu,Hong He
Ce- or La-doped Cu/SSZ-13 catalysts were prepared by a hydrothermal method and Cu, Ce or La ions were incorporated through stepwise ion exchange. The catalyst activity was measured for the ammonia selective catalytic reduction reaction. The structure and composition of catalyst were characterized by using X-ray diffraction, scanning electron microscopy, inductively coupled plasma mass spectrometry solid-state NMR, NH 3 -TPD techniques, and the active components were examined by XPS and XANES . The results indicate that the Ce and La doping can both completely preserve the SCR activity of Cu/SSZ-13 above 300 °C, but there is also a decrease of activity below 200 °C. On the other hand, Ce doping is beneficial to the formation of framework aluminum , stabilizes molecular sieve framework and Cu active sites of Cu/SSZ-13, thereby improves the catalyst hydrothermal stability. But La doping will decrease the amount of framework aluminum and Cu active sites of Cu/SSZ-13 after hydrothermally aging, even destroy zeolite CHA structure. This is quite harmful to the catalyst hydrothermal stability.
研究领域:
催化
·
环境化学
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Zhan Shu,Cencen Zhang,Lizhao Yan,Haoqi Lei,Caixing Peng,Shuang Liu,Lihong Fan,Yingying Chu
Repair of periodontal and maxillofacial bone defects is a major challenge in clinical. Guided bone regeneration (GBR) is considered one of the most effective methods. However, the efficacy of currently available GBR membranes for repair is frequently limited by their poor osteogenic potential and lack of antibacterial activity. The first step in this investigation was to construct a zinc-based zeolite-imidazolate framework loaded with copper ions ( [email protected] ). Following that, a novel polycaprolactone/polylactic acid/nano-hydroxyapatite/ [email protected] (PCL/PLA/n-HA/ [email protected] ) GBR membrane was developed using a simple porogen with nonsolvent-induced phase separation (NIPS) approach. The produced membrane with asymmetric porous structure (one smooth side and one rough side) possesses hydrophilicity corresponding to the roughness of its two sides. The superior mechanical property, stability of degradation, and ion release capability of the membrane all contribute to the clinical feasibility. Additionally, in vitro biological experiments demonstrated that the PCL/PLA/n-HA/ [email protected] membrane had favorable osteogenic and antibacterial properties, which suggests the high potential for application in the GBR procedure.
研究领域:
牙科材料
·
生物材料
·
组织工程
·
生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
Open Chemistry
·
2020
·Vol. 18
·期 1
·97-107
·
IF 1.216
Huayu Huang,Yang Wang,Yubin Zhang,Zhiying Niu,Xinli Li
Amino-functionalized graphene oxide (GO-NH 2 ) was synthesized by grafting (3-aminopropyl) triethoxysilane on the graphene oxide (GO) surface. The GO-NH 2 with high surface area and numerous active sites can efficiently adsorb Cr(VI), Cu(II), Pb(II) and Cd(II) ions. The maximum adsorption capacities of GO-NH 2 for Cr(VI), Cu(II), Pb(II) and Cd(II) were 280.11, 26.25, 71.89 and 10.04 mg g −1 , respectively. The pseudo-first-order and pseudo-second-order kinetic models were employed to describe the kinetic processes. The experimental data agreed well with the pseudo-second-order kinetic equation, and the adsorption of heavy metals onto GO-NH 2 occurs via chemical adsorption. The characteristics of Cr(VI), Cu(II), Pb(II) and Cd(II) in the GO-NH 2 adsorption processes were analyzed using the Langmuir and Freundlich isotherm models. The adsorption processes of Pb(II) and Cd(II) on GO-NH 2 were fit by the Langmuir model. The Freundlich isotherm model was well correlated to Cr(VI) and Cu(II). The GO-NH 2 is a promising material for the removal of heavy metal ions from industrial wastewater. This study provides an effective pathway to process industrial wastewater, and the GO-NH 2 has a good adsorption effect for the treatment of heavy metals in industrial wastewater.
研究领域:
环境科学
·
化学工程
·
材料科学
·
水处理
✓ 已验证
DOI
高影响因子