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Active site identification and engineering during the dynamic evolution of copper-based catalysts for electrocatalytic CO_(2) reduction

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Science China Chemistry 2023年第1期66卷 78-95页

作者： Bangwei Deng Xueyang Zhao Yizhao Li Ming Huang Shihan Zhang Fan Dong Yangtze Delta Region Institute(Huzhou) University of Electronic Science and Technology of ChinaHuzhou 313001China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731China Key Laboratory of Microbial Technology for Industrial Pollution Control of Zhejiang Province College of EnvironmentZhejiang University of TechnologyHangzhou 310014China

To date,copper-based catalysts are one of the most prominent catalysts that can electrochemically reduce CO_(2)towards highvalue fuels or chemicals,such as ethylene,ethanol,and acetic ***,the chemically active feature of Cu-based catalysts hinders the understanding of the intrinsic catalytic active sites during the initial and the operative processes of electrochemical CO_(2)reduction(CO_(2)RR).The identification and engineering of active sites during the dynamic evolution of catalysts are thereby vital to further improve the activity,selectivity,and durability of Cu-based catalysts for high-performance CO_(2)*** this regard,four triggers for the dynamic evolution of catalysts were introduced in ***,three typical active-site theories during the dynamic reconstruction of catalysts were *** addition,the strategies in catalyst design were summarized according to the latest reports of Cu-based catalysts for CO_(2)RR,including the tuning of electronic structure,controlling of the external potential,and regulation of local catalytic ***,the conclusions and perspectives were provided to inspire more investigations and studies on the intrinsic active sites during the dynamic evolution of catalysts,which could promote the optimization of the catalyst system to further improve the performance of CO_(2)RR.

关键词： active site dynamic reconstruction copper-based catalysts electrochemical CO_(2)reduction local catalytic environment

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Effect of preparation methods of aluminum emulsions on catalytic performance of copper-based catalysts for methanol synthesis from syngas

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Journal of Natural Gas Chemistry 2010年第5期19卷 487-492页

作者： Lili Wang Wen Ding Yingwei Liu Weiping Fang Yiquan Yang Department of Chemical and Biochemical Engineering College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 Fujian China Department of Chemistry College of Chemistry and Chemical Engineering and National Engineering Laboratory for Green Chemical Productions of Alcohols Ethers and Esters Xiamen University Xiamen 361005 Fujian China

Various Cu/ZnO/Al2O3 catalysts have been synthesized by different aluminum emulsions as aluminum sources and their pertormances tor methanol synthesis from syngas have been investigated. The influences of preparation methods of aluminum emulsions on physicochemical and catalytic properties of catalysts were studied by XRD, SEM, XPS,N2 adsorption-desorption techniques and methanol synthesis from syngas. The preparation methods of aluminum emulsions were found to influence the catalytic activity, CuO crystallite size, surface area and Cu0 surface area and reduction process. The results show that the catalyst CN using the aluminum source prepared by addition the ammonia into the aluminum nitrate （NP） exhibited the best catalytic performance for methanol synthesis from syngas.

关键词： aluminum emulsion copper-based catalysts methanol synthesis Cu+/Cu0

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Catalytic combustion of methane over nano ZrO_2-supported copper-based catalysts

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Chinese Chemical Letters 2007年第8期18卷 993-996页

作者： Fen Fen Qua Wei Chu Li Min Shi Mu Hua Chen Jin Yan Hu Department of Environmental Science and Engineering Sichuan University Chengdu 610065 China Department of Chemical Engineering Sichuan University Chengdu 610065 China

The nano ZrO2-supported copper-based catalysts for methane combustion were investigated by means of N2 adsorption, TEM, XRD, H2-TPR techniques and the test of methane oxidation. Two kinds of ZrO2 were used as support, one （ZrO2-1） was obtained from the commercial ZrO2 and the other （ZrO2-2） was issued from the thermal decomposition of zirconium nitrate. It was found that the CuO/ZrO2-2 catalyst was more active than CuO/ZrO2-1. N2 adsorption, H2-TPR and XRD measurements showed that larger surface area, better reduction property, presence of tetragonal ZrO2 and higher dispersion of active component for CuO/ZrO2-2 than that of CuO/ZrO2-1. These factors could be the dominating reasons for its higher activity for methane combustion.

关键词： Nano ZrO2 copper-based catalysts Catalytic combustion Methane

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One-dimensional Cu-based catalysts with layered Cu-Cu20-CuO walls for the Rochow reaction

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Nano Research 2016年第5期9卷 1377-1392页

作者： Jing Li Zailei Zhang Yongjun Ji Zheying Jin Shanying Zou Ziyi Zhong Fabing Su State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 1 O0190 China University of Chinese Academy of Sciences Beijing 100049 China School of Chemical & Biomedical Engineering Nanyang Technological University (NTU) Singapore 637459 Singapore

A series of copper catalysts with a core-shell or tubular structure containing various contents of Cu, Cu2O, and CuO were prepared via controlled oxidation of Cu nanowires （NWs） and used in the synthesis of dimethyldichlorosilane （M2） via the Rochow reaction. The Cu NWs were prepared from copper （Ⅱ） nitrate using a solution-based reduction method. The samples were characterized by X-ray diffraction, thermogravimetric analysis, temperature-programmed reduction, X-ray photoelectron spectroscopy, transmission electron microscopy, and scanning electron microscopy. It was found that the morphology and composition of the catalysts could be tailored by varying the oxidation temperature and time. During the gradual oxidation of Cu NWs, the oxidation reaction inflated on the outer surface and gradually developed into the bulk of the NWs, leading to the formation of catalysts with various structures and layered compositions, e.g., Cu NWs with surface Cu2O, ternary Cu-Cu2O-CuO core-shell NWs, binary Cu2O-CuO nanotubes （NTs）, and single CuO NTs. Among these catalysts, ternary Cu-Cu2O-CuO core-shell NWs exhibited superior M2 selectivity and Si conversion in the Rochow reaction. The enhanced catalytic performance was mainly attributed to improved mass and heat transfer resulting from the peculiar heterostructure and the synergistic effect among layered components. Our work indicated that the catalytic property of Cu-based nanoparticles can be improved by carefully controlling their structures and compositions.

关键词： controlled oxidation nanowires core-shell structure nanotubes copper-based catalysts Rochow reaction

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Promotional effect of CeO_2 and Y_2O_3 on CuO/ZrO_2 catalysts for methane combustion

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Journal of Rare Earths 2012年第2期30卷 123-127页

作者：黄亮张兴旺陈琳雷乐成 Institute of Industrial Ecology and Environment Yuquan CampusZhejiang University School of Chemistry and Environmental Science Guizhou University for Nationalities

Catalytic combustion of methane was conducted by using a Cu-based catalyst prepared by the plasma-assisted impregnation method. The properties of the catalysts were surveyed by X-ray diffraction （XRD）, X-ray photoelectron spectroscopy （XPS） and temperature-programmed reduction （H2-TPR）. The results showed that the activity of CuO/ZrO2 with the CeO2 and Y2O3 was obviously increased compared with the CuO/ZrO2 catalyst, which was examined in relation to the structure and surface characteristics and might be correlated with their surface oxygen species and redox properties. Among the investigated catalysts, the Ce-CuO/ZrO2 sample exhibited the highest activity for methane combustion.

关键词： copper-based catalysts cerium yttrium catalytic combustion rare earths

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Origin and effect of surface oxygen-containing species on electrochemical CO or CO_(2) reduction reactions

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Science China Chemistry 2023年第1期66卷 96-106页

作者： Xiaoxia Chang Ming He Qi Lu Bingjun Xu College of Chemistry and Molecular Engineering Peking UniversityBejing 100871China Department of Chemical Engineering Tsinghua UniversityBejing 100084China

Renewable-energy-powered electrochemical CO or CO_(2)reduction reactions(CO_(2)RR)provide one of the most promising strategies to upgrade CO_(2)to valuable *** the past decade,the existence and the mechanistic role of oxygen-containing species,such as(sub)surface oxide,hydroxide and oxyhydroxide species,at the electrode–electrolyte interface under reductive conditions have emerged as a topic of acute discussion within the CO_(2)RR ***-derived Cu attracted the most attention,while other surfaces,including Au,Ag and Sn,were also widely *** review identifies likely causes for contrasting results and views in the literature,summarizes possible oxygen sources for the interfacial oxygen-containing species at the CO_(2)RR conditions,and discusses potential roles these species could play in affecting the rate and product ***,perspectives on future efforts to reveal the identity and role of oxygen-containing species in the CO_(2)RR are presented.

关键词： electrochemical CO_(2)reduction surface oxygen-containing species copper-based catalysts

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Thermodynamics of glycerol hydrogenolysis to propanediols over supported copper clusters: Insights from first-principles study

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Science China Chemistry 2013年第6期56卷 763-772页

作者： GUAN Jing WANG XiCheng WANG XiaoYan MU XinDong Key Laboratory of Biofuels Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of Sciences

copper catalysts supported on metal oxides display unique efficiency and selectivity in catalyzing glycerol hydrogenolysis to propanediols. Understanding the reaction at the molecular level is the key to rational design of better catalysts for propanediol synthesis, which is one of the major challenges for glycerol application in energy. In this work, extensive calculations based on periodic density functional theory were carried out to study thermodynamics of glycerol hydrogenolysis over binary model catalysts, including Cu/ZrO2 and Cu/MgO, with the focus to elucidate the competitive reaction pathways to produce the 1,2-propanediol (1,2-PDO) and 1,3-propanediol (1,3-PDO). Our results suggest that the reaction starts with glycerol dehydration on the metal oxide, followed by sequential hydrogenation over metal centers. based on our explorations on the stabilities of adsorbed reactants, dehydrated intermediates and hydrogenated species along the reaction channels, the DFT calculations show that the 1,2-PDO formation will dominate in comparison to the 1,3-PDO from thermodynamic viewpoint. This is consistent with our experiments where the Cu catalysts seem to give the 1,2-PDO as a main product. The calculations and experiments also indicate that the Cu/MgO exhibits superior activities than Cu/ZrO2 for the hydrogenolysis of glycerol molecules.

关键词： density functional calculations glycerol hydrogenolysis propanediols copper-based catalysts mechanism

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