期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 6, 期 14, 页码 5668-5683出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6cy00335d
关键词
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资金
- JSPS KAKENHI [26249121]
- [263554]
- Grants-in-Aid for Scientific Research [26249121, 14J03554] Funding Source: KAKEN
A Re-Pd/SiO2 (Re/Pd = 8) catalyst was applied to hydrogenation of dicarboxylic acids (succinic acid, glutaric acid and adipic acid) to diols. In the hydrogenation of dicarboxylic acids, ex situ liquid-phase (in only 1,4-dioxane solvent) reduced Re-Pd/SiO2 showed much higher activity than in situ liquid-phase (in the mixture of dicarboxylic acid and 1,4-dioxane) and gas-phase reduced ones, in which the in situ liquid-phase reduced catalyst has been reported to show good activity in the hydrogenation of monocarboxylic acids. High diol yields (71-89%) were achieved in the hydrogenation of dicarboxylic acids on the ex situ liquid-phase reduced catalyst at 413 K. Lactones and hydroxycarboxylic acids were first formed as intermediates in the reaction of C4-C5 and >= C6 dicarboxylic acids, respectively. Characterization using XRD, XPS and XAS indicates that ex situ liquid-phase reduced catalysts with high activity contains comparable amounts of Re-0 and Ren+ species, both of which have been reported to be necessary for good performance. The amount of Ren+ species on the in situ liquid-phase reduced catalysts is much larger than that of surface Re-0 species. This result suggests that the presence of dicarboxylic acids suppresses the reduction of Re species to Re-0 on the calcined catalysts while that of monocarboxylic acids does not, which leads to the low activity in the hydrogenation of dicarboxylic acids on in situ liquid-phase reduced catalysts.
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