期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 296, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120333
关键词
Supported Pt catalyst; Residual chloride; Soft Lewis acid; Isomerization reaction; Allylic esters
资金
- ALCA program from the Japan Science and Technology Agency [11102798]
- Mitsubishi Chemical Corporation
The study demonstrates that highly dispersed supported platinum catalyst can act as a heterogeneous soft Lewis acid, showing high turnover numbers and reusability in the isomerization of allylic esters under solvent-free conditions. The residual chloride anion enhances the Lewis acidity of the Pt metal center, improving catalytic activity.
Heterogeneous acid and base catalysts play a crucial role in many important chemical processes. Hard Lewis and Bronsted acid catalysts like silica-alumina and zeolites have been widely applied in numerous reactions; however, developing reusable and active soft Lewis acid catalysts remain a challenge. Herein, we demonstrate for the first time that a highly dispersed supported platinum catalyst can act as a heterogeneous soft Lewis acid. High turnover numbers and reusability were observed in the isomerization of allylic esters under solvent-free conditions. Moreover, the as-prepared catalysts are characterized by X-ray photoelectron spectroscopy (XPS) and Xray absorption fine structure (XAFS), revealing that the highly dispersed Pt clusters with Pt-Cl bonds play a key role in the high activity. The residual chloride anion enhances the Lewis acidity of the Pt metal center and thus improves the catalytic activity. Simultaneously, the high catalytic activity of Pt/CeO2 with residual chloride and the soft Lewis acid mechanism are also proved by density functional theory (DFT) calculations based on the model reaction.
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