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CO气相氧化偶联制草酸二乙酯催化剂研究
引用本文:王保伟,许根慧,马新宾,何菲,韩森.CO气相氧化偶联制草酸二乙酯催化剂研究[J].燃料化学学报,2000,28(3):262-267.
作者姓名:王保伟  许根慧  马新宾  何菲  韩森
作者单位:1. 天津大学化工学院,天津大学,天津,300072
2. 天津大学一催化工国家重点实验室
基金项目:国家计委“九五”科技攻关项目
摘    要:利用化学吸附仪、XRD、XPS、EPMA、SEM等技术,对CO气相偶联制草酸二乙酸催化剂的比表面,孔分布,晶相,反应前后催化剂活性组分在表面和中心的价态对比及活性组分与助剂的分布进行了分析表征和反应机理探讨。研究表明小比表面大孔径的率剂反应效果好,在整个反应过程中催化剂活性组分Pd元素Pd=Pd^+2,通过与亚硝酸乙酯及CO的反应来改变Pd的价态,反应过程中催化剂的成分变化和迁移与氧化还原“共催化

关 键 词:催化剂  孔结构  乙酸二乙酯  一氧化碳  氧化

STUDY OF CATALYST OF CO COUPLING TO DIETHYL OXALATE IN GASEOUS PHASE
WANG Bao-wei,XU Gen-hui,MA Xin-bin,HE Fei,HAN Sen.STUDY OF CATALYST OF CO COUPLING TO DIETHYL OXALATE IN GASEOUS PHASE[J].Journal of Fuel Chemistry and Technology,2000,28(3):262-267.
Authors:WANG Bao-wei  XU Gen-hui  MA Xin-bin  HE Fei  HAN Sen
Abstract:The gaseous phase synthesis of diethyl oxalate and oxalic acid with CO was an important project of C 1 chemical technology The catalysts of the process of diethyl oxalate preparing by CO coupling reaction in gaseous phase were analyzed with the chemical absorbed apparatus of CHEMBET-3000 for the specific surface area and the pore volume and the pore size distribution, XRD for the catalytic crystal structure, XPS for the variation of valence of active constituent and SEM for the distribution of the active constituent before and after reaction The reaction mechanism was discussed The results indicated that the catalyst with smaller specific surface area and bigger pore size was better one The valence of the active constituent Pd changed from Pd 0 to Pd 2 and then Pd 2 to Pd 0 through red-ox mechanism Pd was oxidized by C 2H 5ONO and reduced by CO during the course of reaction The variation of valence and migration of active constituent agreed with the "catalytic circulation" mechanism
Keywords:diethyl oxalate  catalyst  specific surface area  pore volume and size distribution  mechanism
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