TY - JOUR
T1 - Reaction-driven surface reconstruction of ZnAl2O4 boosts the methanol selectivity in CO2 catalytic hydrogenation
AU - Zhang, Xinbao
AU - Zhang, Guanghui
AU - Liu, Wei
AU - Yuan, Fei
AU - Wang, Jianyang
AU - Zhu, Jie
AU - Jiang, Xiao
AU - Zhang, Anfeng
AU - Ding, Fanshu
AU - Song, Chunshan
AU - Guo, Xinwen
N1 - Funding Information:
This work was financially supported by the National Key Research and Development Program of China (2016YFB0600902-4), National Natural Science Foundation of China (21902019), and the Fundamental Research Funds for the Central Universities (DUT20RC(5)002). X.J. acknowledges the financial support from the Center for Understanding the Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME), an Energy Frontier Research Center funded by U.S. Department of Energy, Office of Science, Basic Energy Sciences. We also thank Prof. Zhaochi Feng of Dalian Institute of Chemical Physics and Mr. Yanli Wang of Dalian University of Technology for assistance in Raman characterization.
Funding Information:
This work was financially supported by the National Key Research and Development Program of China ( 2016YFB0600902-4 ), National Natural Science Foundation of China ( 21902019 ), and the Fundamental Research Funds for the Central Universities ( DUT20RC(5)002 ). X.J. acknowledges the financial support from the Center for Understanding the Control of Acid Gas-Induced Evolution of Materials for Energy (UNCAGE-ME) , an Energy Frontier Research Center funded by U.S. Department of Energy, Office of Science, Basic Energy Sciences . We also thank Prof. Zhaochi Feng of Dalian Institute of Chemical Physics and Mr. Yanli Wang of Dalian University of Technology for assistance in Raman characterization.
Publisher Copyright:
© 2020 Elsevier B.V.
PY - 2021/5/5
Y1 - 2021/5/5
N2 - Identifying the surface structure of heterogeneous catalysts is critical for understanding the active sites, but it remains challenging due to the difficulty in characterizing the catalytic surfaces especially at elevated temperatures. Zn-based catalysts are high-efficiency alternatives for high-temperature methanol synthesis from CO2, as well as in bifunctional catalysts for hydrocarbons synthesis. Herein, the surface reconstruction of ZnAl2O4 spinel during CO2 hydrogenation reaction was investigated using detailed spectroscopic characterization. The results indicate that the reaction-driven surface reconstruction leads to the formation of amorphous ZnO on the ZnAl2O4 surface, which is accompanied by the increasing catalytic activity for methanol production. Kinetic analysis, STEM and in situ FTIR results indicate that the amorphous ZnO boosts the methanol formation rate by promoting the activation of H2. This study provides useful insight into the structure-activity relationship of zinc-based catalysts for CO2 hydrogenation and future design of new catalysts.
AB - Identifying the surface structure of heterogeneous catalysts is critical for understanding the active sites, but it remains challenging due to the difficulty in characterizing the catalytic surfaces especially at elevated temperatures. Zn-based catalysts are high-efficiency alternatives for high-temperature methanol synthesis from CO2, as well as in bifunctional catalysts for hydrocarbons synthesis. Herein, the surface reconstruction of ZnAl2O4 spinel during CO2 hydrogenation reaction was investigated using detailed spectroscopic characterization. The results indicate that the reaction-driven surface reconstruction leads to the formation of amorphous ZnO on the ZnAl2O4 surface, which is accompanied by the increasing catalytic activity for methanol production. Kinetic analysis, STEM and in situ FTIR results indicate that the amorphous ZnO boosts the methanol formation rate by promoting the activation of H2. This study provides useful insight into the structure-activity relationship of zinc-based catalysts for CO2 hydrogenation and future design of new catalysts.
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U2 - 10.1016/j.apcatb.2020.119700
DO - 10.1016/j.apcatb.2020.119700
M3 - Article
AN - SCOPUS:85097238869
SN - 0926-3373
VL - 284
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
M1 - 119700
ER -