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selective oxidation of methanol to dimethoxymethane over V_2O_5/Ti O_2–Al_2O_3 catalysts

Science Bulletin 2015年第11期60卷 1009-1018,I0007页

作者：王拓孟亚利曾亮巩金龙 Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin University Collaborative Innovation Center of Chemical Science and Engineering

This paper describes the effect of the prepara- tion method of binary oxide supports （TiO2-Al2O3） on catalytic performance of V2O5/TiO2-Al2O3 catalysts for methanol selective oxidation to dimethoxymethane （DMM）. The TiO2-A1203 supports are synthesized by a number of methods including mechanical mixing, ball milling, precipitation, co-precipitation, and sol-gel method, which is followed by incipient wetness impregnation to produce V2O5/TiO2-Al2O3 catalysts. Among these samples, the V2O5/TiO2-Al2O3 catalyst prepared by the sol-gel method has the best catalytic performance with a maximum methanol conversion of 48.9 % and a high DMM selectivity of 89.9 % at 393 K, showing superior performance than V2O5/TiO2 and V2O5/Al2O3. The excellent catalytic performance of V2O5/TiO2-Al2O3 is attributed to the effective interaction between the active component and the mixed support. Such interaction changes the chemical states of supported active V components, produces an increased amount of V^4＋ species, and facilitates the electron transfer between support and active component. Additionally, the incorporation of titanium cation into the alumina structure could also help produce an appropriate amount of acidic sites, which increases the DMM selectivity. The coordinated environment of the dispersed vanadia on TiO2-Al2O3 mixed support improves the catalytic efficiency on methanol oxidation to DMM.

关键词： methanol selective oxidation Dimethoxymethane V2O5/TiO2-Al2O3 Binary oxide support

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Coordination Effect-Promoted Durable Ni(OH)_(2) for Energy-Saving Hydrogen Evolution from Water/ methanol Co-Electrocatalysis

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Nano-Micro Letters 2022年第12期14卷 176-194页

作者： Guodong Fu Xiaomin Kang Yan Zhang Xiaoqiang Yang Lei Wang Xian-Zhu Fu Jiujun Zhang Jing-Li Luo Jianwen Liu Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China School of Mechanical Engineering University of South ChinaHengyang 421001Hunan ProvincePeople’s Republic of China Institute for Sustainable Energy College of SciencesShanghai UniversityShanghai 200444People’s Republic of China

Electrocatalytic water splitting is a viable technique for generating hydrogen but is precluded from the sluggish kinetics of oxygen evolution reactions(OER).Small molecule oxidation reactions with lower working potentials,such as methanol oxidation reactions,are good alternatives to OER with faster ***,the typically employed Ni-based electrocatalysts have poor activity and ***,a novel three-dimensional(3D)-networking Modoped Ni(OH)_(2) with ultralow Ni-Ni coordination is synthesized,which exhibits a high MOR activity of 100 mA cm^(−2) at 1.39 V,delivering 28 mV dec^(−1) for the Tafel ***,hydrogen evolution with value-added formate co-generation is boosted with a current density of more than 500 mA cm^(−2) at a cell voltage of 2.00 V for 50 h,showing excellent stability in an industrial alkaline concentration(6 M KOH).Mechanistic studies based on density functional the-ory and X-ray absorption spectroscopy showed that the improved performance is mainly attributed to the ultralow Ni-Ni coordination,3D-networking structures and Mo dopants,which improve the catalytic activity,increase the active site density and strengthen the Ni(OH)_(2)3D-networking structures,*** study paves a new way for designing electrocatalysts with enhanced activity and durability for industrial energy-saving hydrogen production.

关键词： Coordination effect methanol selective oxidation NiMoO4 Formate Energy-saving hydrogen production

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