Journal
ACS CATALYSIS
Volume 11, Issue 15, Pages 10014-10019Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c02742
Keywords
in situ characterization; surface intermediates; reaction mechanism; TPSR; DRIFTS
Categories
Funding
- National Natural Science Foundation of China [91945301, 91745202]
- Chinese Academy of Sciences
- Changjiang Scholars Program of Ministry of Education of China
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The study revealed that CO and H-2 activation occurs at the Al and Zn sites of the ZnAl2O4 catalyst, forming active bidentate formate species and reversibly adsorbed hydrogen species. The hydrogenation of resulting bidentate formate species at the Al site is the rate-controlling step with a barrier of 83.8 kJ/mol. These results deepen the understanding of the synergistic catalysis of Al and Zn sites in ZnAl2O4 catalyst and the rate-controlling step in CO hydrogenation to methanol/dimethyl ether.
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.
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