CATALYSIS Active sites for CO2 hydrogenation to methanol on Cu/ZnO catalysts

被引:1325
作者
Kattel, Shyam [1 ]
Ramirez, Pedro J. [2 ]
Chen, Jingguang G. [1 ,3 ]
Rodriguez, Jose A. [1 ,4 ]
Liu, Ping [1 ,4 ]
机构
[1] Div Chem, Brookhaven Natl Lab, Upton, NY 11973 USA
[2] Cent Univ Venezuela, Fac Ciencias, Caracas 1020, Venezuela
[3] Columbia Univ, Dept Chem Engn, New York, NY 10027 USA
[4] SUNY Stony Brook, Dept Chem, Stony Brook, NY 11790 USA
关键词
COPPER; CU; SURFACE; ZNO; CONVERSION; PROMOTION; OXIDE;
D O I
10.1126/science.aal3573
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The active sites over commercial copper/zinc oxide/aluminum oxide (Cu/ZnO/Al2O3) catalysts for carbon dioxide (CO2) hydrogenation to methanol, the Zn-Cu bimetallic sites or ZnO-Cu interfacial sites, have recently been the subject of intense debate. We report a direct comparison between the activity of ZnCu and ZnO/Cu model catalysts for methanol synthesis. By combining x-ray photoemission spectroscopy, density functional theory, and kinetic Monte Carlo simulations, we can identify and characterize the reactivity of each catalyst. Both experimental and theoretical results agree that ZnCu undergoes surface oxidation under the reaction conditions so that surface Zn transforms into ZnO and allows ZnCu to reach the activity of ZnO/Cu with the same Zn coverage. Our results highlight a synergy of Cu and ZnO at the interface that facilitates methanol synthesis via formate intermediates.
引用
收藏
页码:1296 / +
页数:4
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