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贵金属对NM/WO3-ZrO2(NM=Ru,Rh和Pd)催化乙烯直接氧化制乙酸反应的影响(英文) 预览 被引量:2

Influence of Noble Metals on the Direct Oxidation of Ethylene to Acetic Acid over NM/WO_3-ZrO_2 (NM = Ru, Rh, and Pd) Catalysts
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摘要 研究了负载Ru,Rh和Pd的WO3-ZrO2催化剂在乙烯直接氧化制乙酸反应中的催化性能.结果显示,负载的贵金属对催化剂的催化性能有非常重要的影响.Rh/WO3-ZrO2催化剂具有最高的乙烯转化率,而Ru/WO3-ZrO2催化剂对反应几乎没有活性.H2化学吸附结果显示,高的催化性能来源于高的金属分散度.Pd/WO3-ZrO2催化剂显示了最高的乙酸选择性(75%),而其它两个催化剂的乙酸选择性都非常低(~10%).程序升温氧化和程序升温还原结果显示,贵金属–O键的键强对产物的选择性具有重要的影响.弱的贵金属–O键可以通过将氧插入到乙烯和/或乙醛中而有利于乙酸的生成,而强的贵金属–O键会导致乙烯完全氧化为COx. Ru-, Rh-, and Pd/WO3-ZrO2 catalysts were studied for the direct oxidation of ethylene to acetic acid. The catalytic activity and selectivity depended strongly on the noble metals used. Rh/WO3-ZrO2 gave the highest conversion of ethylene, whereas Ru/WO3-ZrO2 was almost inactive. The higher catalytic activity was attributed to a better metal dispersion. Pd/WO3-ZrO2 gave the highest selectivity for acetic acid (75%), with the selectivity of the other two catalysts being rather low (~10%). Temperature-programmed oxidation and H2 reduction experiments were used to show that the strength of the noble metal-oxygen bond played an important role in product distribution. A weak metal--oxygen bond favored the formation of acetic acid, while a strong metal-oxygen bond favored the combustion of ethylene to COx.
作者 王丽霞 徐庶亮 楚文玲 杨维慎 WANG Lixia, XU Shulian, CHU Wenling, YANG Weishen (1.State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China; 2.Graduate University of Chinese Academy of Sciences, Beijing 100049, China)
出处 《催化学报》 SCIE EI CAS CSCD 北大核心 2009年第12期 1281-1286,共6页 Chinese Journal of Catalysis
基金 Supported by the National Science Foundation for Distinguished Young Scholars (20725313) and the National Basic Research Program of China (973 Program, 2005CB221404)
关键词 乙烯 氧化 乙酸 氧化钨 氧化锆 ethylene oxidation acetic acid tungstated zirconia palladium ruthenium rhodium
作者简介 Corresponding author. E-mail: cwl@dicp.ac.cn Corresponding author. Tel: +86-411-84379073; Fax: +86-411-84694447; E-mail: yangws@dicp.ac.cn; URL: http://yanggroup.dicp.ac.cn
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