Mechanistic insights into the effects of support on the reaction pathway for aqueous-phase hydrogenation of carboxylic acid over the supported Ru catalysts

被引：55
作者：
Chen, Lungang [1 ]
Li, YuPing [1 ]
Zhang, Xinghua [1 ]
Zhang, Qi [1 ]
Wang, Tiejun [1 ]
Ma, Longlong [1 ]
机构：
[1] Chinese Acad Sci, Guangzhou Inst Energy Convers, Key Lab Renewable Energy, Guangzhou 510640, Guangdong, Peoples R China
来源：
APPLIED CATALYSIS A-GENERAL | 2014年 / 478卷
基金：
中国国家自然科学基金;
关键词：
Aqueous-phase; Hydrogenation; Ru catalyst; Effect of support; Acyl; Decarbonylation; DRIFTS; ACETIC-ACID; CO ADSORPTION; LACTIC-ACID; RUTHENIUM CATALYSTS; FTIR; H-2; HYDRODEOXYGENATION; HYDROGENOLYSIS; SPECTROSCOPY; REDUCTION;
D O I：
10.1016/j.apcata.2014.03.038
中图分类号：
O64 [物理化学（理论化学）、化学物理学];
学科分类号：
070304 ; 081704 ;
摘要：
Several supported Ru catalysts, Ru/TiO2, Ru/ZrO2, Ru/SiO2, Ru/gamma-Al2O3 and Ru/SiO2-Al2O3, were prepared and investigated for propanoic acid aqueous-phase hydrogenation. H-2-TPR, NH3-TPD, pyridine-FTIR and propanoic acid-DRIFTS techniques were performed to explore the metal-support interaction, acid sites and key adsorption species. The effect of support on the reaction pathway of C=O hydrogenation and decarbonylation of acyl species was discussed. Compared with Ru/ZrO2 and Ru/SiO2 catalysts, high selectivity of C=O hydrogenation was obtained over the catalysts with more Lewis acid sites, such as Ru/gamma-Al2O3 and Ru/SiO2-Al2O3 catalysts. The DRIFTS results suggest that the formation of adsorption species (acyl, carboxylate and carboxylic acid) is strongly depended on the nature of support. The metal-acid bifunctional sites are indispensable for the C=O hydrogenation of acyl. However, the decarbonylation of acyl on the metal sites requires the relatively weak metal-support interaction and few of Lewis acid sites. (C) 2014 Elsevier B.V. All rights reserved.
引用
收藏
页码：117 / 128
页数：12
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