The Cyclopentanone Self-condensation Over Calcined and Uncalcined TiO2-ZrO2 with Different Acidic Properties

被引:6
|
作者
Wan, Jinmeng [1 ]
Yang, Haixia [1 ]
Fu, Lin [1 ]
Lin, Wenjing [1 ]
Hu, Qing [1 ]
Xi, Fengcao [1 ]
Pan, Langsheng [1 ,2 ]
Li, Yongfei [1 ,2 ]
Liu, Yuejin [1 ,2 ]
机构
[1] Xiangtan Univ, Sch Chem Engn, Xiangtan 411105, Peoples R China
[2] Xiangtan Univ, Natl & Local United Engn Res Ctr Chem Proc Simula, Xiangtan 411105, Peoples R China
基金
中国国家自然科学基金;
关键词
Cyclopentanone; TiO2-ZrO2; Aldol condensation; Calcination; Kinetics; ALDOL CONDENSATION; TRANSFER HYDROGENATION; MIXED OXIDES; PHOTOCATALYTIC ACTIVITY; CATALYTIC-ACTIVITY; ELEMENTARY STEPS; ETHYL LEVULINATE; TIO2; ACETALDEHYDE; ACETONE;
D O I
10.1007/s10562-021-03655-z
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
The self-condensation of cyclopentanone has been studied over calcined and uncalcined TiO2-ZrO2. The catalyst properties were examined by XRD, FTIR, SEM, N-2 adsorption-desorption, and pyridine FTIR. Compared with calcined TiO2-ZrO2, uncalcined TiO2-ZrO2 exhibited superior catalytic performance (94% conversion of cyclopentanone and 86% yield of dimer). This might be because uncalcined TiO2-ZrO2 has both Lewis and BrOnsted acids, while calcined TiO2-ZrO2 only contains Lewis acids. Kinetics analysis indicated that C-C coupling was the rate-limiting step on the two catalysts. For uncalcined TiO2-ZrO2, the C-C coupling occurred between the two species on the catalyst surface. Through the H bond, the cyclopentanone was firmly adsorbed on the catalyst surface by BrOnsted acid sites, then the enol intermediate could attack another cyclopentanone polarized by adjacent Lewis acid sites. As a consequence, the coexistence of BrOnsted and Lewis acids in catalysts exhibited enhanced activity in cyclopentanone self-condensation.
引用
收藏
页码:806 / 820
页数:15
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