Synergistic Catalysis of Al and Zn Sites of Spinel ZnAl2O4 Catalyst for CO Hydrogenation to Methanol and Dimethyl Ether

被引：52

作者：

Ye, Aiai ^{[1
,2
]}

Li, Zhaorui ^{[1
,2
]}

Ding, Jieqiong ^{[1
,2
]}

Xiong, Wei ^{[1
,2
]}

Huang, Weixin ^{[1
,2
,3
]}

机构：

[1] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Key Lab Surface & Interface Chem & Energy Catalys, Hefei 230026, Peoples R China

[2] Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Peoples R China

[3] Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China

来源：

ACS CATALYSIS | 2021年 / 11卷 / 15期

基金：

中国国家自然科学基金;

关键词：

in situ characterization; surface intermediates; reaction mechanism; TPSR; DRIFTS; FOURIER-TRANSFORM; SELECTIVE CONVERSION; CARBON-MONOXIDE; LOWER OLEFINS; ADSORPTION; ALUMINA; HYDROXYLS; OXIDATION; PRESSURE; DESIGN;

D O I：

10.1021/acscatal.1c02742

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：

Activation and surface reactions of CO and H-2 on spinel ZnAl2O4 catalyst under CO hydrogenation reaction conditions were studied using temperature-programmed surface reaction spectra and in situ diffuse reflectance Fourier transform infrared spectroscopy. CO and H-2 activation was found to occur at the Al and Zn sites of ZnAl2O4 catalyst to form active bidentate formate species and reversibly adsorbed hydrogen species for methanol/diemthyl etherproduction, respectively. The hydrogenation of resulting bidentate formate species at the Al site is the rate-controlling step and exhibits a barrier of 83.8 kJ/mol. These results reveal the synergistic catalysis of Al and Zn sites of spinel ZnAl2O4 and rate-controlling step in catalyzing CO hydrogenation to methanol/dimethyl ether, which greatly deepens fundamental understanding of oxides-catalyzed CO hydrogenation reaction.

引用

页码：10014 / 10019

页数：6

共 40 条

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