文献类型：期刊文献

英文题名：Dual functions of CoOx decoration in PtCo/CeO2 catalysts for the hydrogen-borrowing amination of alcohols to primary amines

作者：Tong, Tao[1,2];Guo, Wanjun[1,2];Liu, Xiaohui[1,2];Guo, Yong[1,2];Pao, Chih-Wen[3];Chen, Jeng-Lung[3];Hu, Yongfeng[4];Wang, Yanqin[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai Key Lab Funct Mat Chem, Meilong Rd 130, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, Meilong Rd 130, Shanghai 200237, Peoples R China;[3]Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan;[4]Canadian Light Source Inc, 44 Innovat Blvd, Saskatoon, SK S7N 2V3, Canada

年份：2019

卷号：378

起止页码：392

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20193907477460);WOS:【SCI-EXPANDED(收录号:WOS:000494887100043)】；

基金：This work was supported financially by the NSFC of China (No. 21872050, 21832002, 21808063), the Fundamental Research Funds for the Central Universities (222201718003) and the Science and Technology Commission of Shanghai Municipality (18ZR1408500, 10dz2220500). The authors declare no competing financial interest.

语种：英文

外文关键词：Pt-based bimetallic catalysis; Hydrogen borrowing; Primary amines; CoOx additive; Geometric effect

摘要：Amines, especially primary amines, are value-added fine chemicals widely used,in modern industries. Here, a PtCo/CeO2 catalyst is designed for the hydrogen-borrowing amination of alcohols, especially the conversion of cyclopentanol to cyclopentanylamine. CoOx decoration over Pt/CeO2 is able to enhance both selectivity to primary amine and catalytic activity. These CoOx species play two roles in alcohol amination, enhancing alcohol dehydrogenation and inhibiting overhydrogenation of a Schiff base intermediate (cyclopentyl cyclopentylidene amine). Comprehensive characterization demonstrates that promotional effects of the CoOx additive have two causes: (1) CoOx species provide an additional Pt-CoO interface for the rate-determining dehydrogenation step; (2) CoOx species block low-coordinated Pt sites for H-2 activation in the overhydrogenation of the Schiff base intermediate, thus suppressing the formation of undesirable secondary amines. This work provides an in-depth understanding of the role of the CoOx additive in PtCo/CeO2 and new insights into the design of Pt-based catalysts for primary amine production via hydrogen-borrowing amination. (C) 2019 Elsevier Inc. All rights reserved.