期刊
JOURNAL OF CATALYSIS
卷 407, 期 -, 页码 149-161出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2022.01.032
关键词
Gallium; CO2; Methanol; Copper; Spectroscopy; Ga3+-doped ZnO
资金
- Spanish Ministry of Science, Innovation and Universities [SEV-2016-0683, RTI2018-099668-B-C21, MAT201784118-C2-1-R]
- Spanish Government (MINECO) [BES-2015-075748]
- CAPES [13191/13-6]
This study presents a detailed understanding of the interactions among the active components in gallium promoted Cu/ZnO catalysts, depending on the speciation of the gallium, and their effect in the CO2 hydrogenation to methanol. The promoting effect of Ga3+-doped in the wurtzite ZnO lattice is compared to that of a zinc gallate phase. It is found that the Ga3+-doped ZnO sample exhibits a strong inhibition of CO formation and an enhanced methanol formation, particularly under conditions where the reverse water gas shift reaction predominates. The catalytic performance is correlated with the microstructure of the catalyst, including a surface enrichment with reduced ZnOx species, stabilization of positive charged copper species, and an increase in the amount of surface basic sites for CO2 adsorption.
A detailed understanding of the interactions among the active components in gallium promoted Cu/ZnO catalysts, depending on the speciation of the gallium, are reported using in situ/operando spectroscopic studies, and their effect in the CO2 hydrogenation to methanol unraveled. In this contribution, the promoting effect of Ga3+-doped in the wurtzite ZnO lattice of a Cu/ZnO/Ga2O3 catalyst is compared to that of a zinc gallate (ZnGa2O4) phase. Remarkably, a strong inhibition of CO formation, together with an enhanced methanol formation, are observed in the Ga3+-doped ZnO sample, specifically at conditions where the competitive reverse water gas shift reaction predominates. The catalytic performance has been correlated with the microstructure of the catalyst where a surface enrichment with reduced ZnOx species, together with the stabilization of positive charged copper species and an increase in the amount of surface basic sites for CO2 adsorption are observed on the most selective sample. (C) 2022 The Author(s). Published by Elsevier Inc.
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