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	氧化锆负载氧化钌催化甲醇低温选择氧化合成甲酸甲酯的活性催化剂结构; Active Structure of Zirconia-Supported Ruthenium Oxide Catalyst for Low-Temperature Oxidation of Methanol to Methyl Formate
	李为臻 ; 刘海超
	2006
关键词	甲醇 选择氧化 甲酸甲酯 氧化锆 氧化钌 负载型催化剂 结构效应 methanol selective oxidation methyl formate zirconia ruthenium oxide supported catalyst structural effect
英文摘要	采用ZrO2负载的RuOx催化剂在低温(如373 K)下催化甲醇选择氧化合成甲酸甲酯,发现RuOx的结构可显著影响反应速率和产物选择性.在相近的甲醇转化率下,RuO42-物种的催化活性和对甲酸甲酯的选择性明显高于RuO2物种,表明在ZrO2表面构筑高活性高选择性的RuO42-结构有利于获得高的甲酸甲酯产率.; The oxidation of methanol to methyl formate at low temperature (373 K) over the ZrO2-supported RuOx catalyst was studied. The methanol oxidation rate and product selectivity strongly depend on the RuOx structure, which is changed in the Ru surface density range of 0.2-3.8 Ru/nm(2). The RuOx structure evolves from isolated RuO42- species below 0.4 Ru/nm(2) to RuO2 clusters above 1.9 Ru/nm(2). Such structural evolution with increasing Ru surface density leads to a decrease in the methanol oxidation rate on per Ru atom and on per exposed Ru atom (i.e. turnover rate). This reveals that RuO42- species are more reactive than RuO2 species, which is consistent with the higher reducibility of the RuO42- structure. These RuO42- species are also more selective than the RuO2 species for the methyl formate formation at similar methanol conversion; a similar to 96% methyl formate selectivity (at similar to 15% methanol conversion) was attained at 0.2 Ru/nm(2) with predominant RuO42- structure. These findings suggest that the highly active and selective RuO42- structure is required for achieving high methyl formate productivity.; 国家自然科学基金; 教育部留学回国人员科研启动基金; 教育部跨世纪优秀人才培养计划; http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000241931800002&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=8e1609b174ce4e31116a60747a720701 ; SCI(E); 中文核心期刊要目总览(PKU); 中国科技核心期刊(ISTIC); 中国科学引文数据库(CSCD); 3; 10; 840-842; 27
语种	中文
出处	SCI ; 万方 ; http://d.g.wanfangdata.com.cn/Periodical_cuihuaxb200610002.aspx
出版者	催化学报
内容类型	其他
源URL	[http://hdl.handle.net/20.500.11897/80488]
专题	化学与分子工程学院
推荐引用方式 GB/T 7714	李为臻,刘海超. 氧化锆负载氧化钌催化甲醇低温选择氧化合成甲酸甲酯的活性催化剂结构, Active Structure of Zirconia-Supported Ruthenium Oxide Catalyst for Low-Temperature Oxidation of Methanol to Methyl Formate. 2006-01-01.

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