Catalyst consisting of Ag nanoparticles anchored on amine-derivatized mesoporous silica nanospheres for the selective hydrogenation of dimethyl oxalate to methyl glycolate

被引:34
作者
Dong, Guilin [1 ]
Cao, Yueqiang [2 ]
Zheng, Sainan [3 ]
Zhou, Jinghong [2 ]
Li, Wei [1 ]
Zaera, Francisco [4 ,5 ]
Zhou, Xinggui [2 ]
机构
[1] East China Univ Sci & Technol, Sch Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China
[2] East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China
[3] Pujing Chem Ind Co Ltd, 166 Minhong Rd, Shanghai 201102, Peoples R China
[4] Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA
[5] Univ Calif Riverside, UCR Ctr Catalysis, Riverside, CA 92521 USA
基金
美国国家科学基金会; 国家重点研发计划;
关键词
DMO hydrogenation; Methyl glycolate; Surface amination; Confinement; Silver catalyst; CHEMOSELECTIVE HYDROGENATION; SILVER NANOPARTICLES; ETHYLENE-GLYCOL; AG/SIO2; CATALYST; PERFORMANCE; TEMPERATURE; CARBON; NANOCUBES; NM; CU;
D O I
10.1016/j.jcat.2020.08.018
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
Developing efficient catalysts for the selective hydrogenation of dimethyl oxalate (DMO) is of great significance for the coal-based production of methyl glycolate (MG), but designing processes for this conversion is challenging. Herein we report an unprecedented catalytic performance for the selective hydrogenation of DMO to MG, achieved by using a catalyst based on Ag nanoparticles anchored inside the mesopores of amine-derivatized silica nanospheres (NH2-MSNS). It was determined that the unique microenvironment endowed by the amine-derivatized channel surfaces helps this Ag catalyst promote the activation of DMO and H-2 to yield MG with high selectivity, and also prevents sintering and coking, hence improving stability. Accordingly, the resulting Ag/NH2-MSNS catalyst was shown to be capable of promoting the hydrogenation reaction with a turnover frequency of 230 h(-1) and a MG selectivity of 97% at nearly 100% of DMO conversion, a performance that was sustained for at least 250 h; these results are significantly better than those seen with other reported catalysts. Our study points to a promising route for the development of high-performing Ag catalysts to be used in the coal-based MG production. (C) 2020 Elsevier Inc. All rights reserved.
引用
收藏
页码:155 / 162
页数:8
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