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Active copper structures in ZnO-Cu interfacial catalysis: CO2 hydrogenation to methanol and reverse water-gas shift reactions

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Abstract

Cu-ZnO-based catalysts are widely used to catalyze the CO2 hydrogenation to methanol and reverse water-gas shift (RWGS) reactions. Herein, via a combined experimental and theoretical calculation study of various Cu nanocrystals (NCs) with well-defined Cu facets and corresponding ZnO/Cu NC inverse catalysts, we demonstrate the Cu{110} facets as the most active facet for ZnO-Cu interfacial catalysis in the CO2 hydrogenation to methanol with an apparent activation energy as low as 25.3±3 kJ mol−1 and the Cu{100} facets as the most active facet for both ZnO-Cu interfacial catalysis and Cu catalysis in the RWGS reaction. Although the ZnO-Cu interface is more active in catalyzing the RWGS reaction than the Cu surface, the RWGS reaction occurs mainly on the bare Cu surface of ZnO/Cu inverse catalysts under the CO2 hydrogenation to methanol instead of that at the ZnO-Cu interface. This fundamental understanding will greatly help to fabricate efficient Cu-ZnO-based catalysts for the CO2 hydrogenation to methanol.

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Acknowledgements

This work was financially supported by the National Key R&D Program of China (2022YFA1504601, 2021YFA1502804). the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0450102), the National Natural Science Foundation of China (91945301, 92145302, U1930203 and 22011530114), the Fundamental Research Funds for the Central Universities (20720220008) and the Changjiang Scholars Program of the Ministry of Education of China. The authors thank the Hefei Advanced Computing Center.

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  1. These authors contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory of Precision and Intelligent Chemistry, iChEM, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China

    Wei Xiong, Xuanye Chen, Jieqiong Ding, Aiai Ye, Wenhua Zhang & Weixin Huang

  2. Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China

    Zongfang Wu

  3. Research Institute of Applied Chemistry, Jiangxi Academy of Sciences, Nanchang, 330096, China

    Xuanye Chen

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  1. Wei Xiong
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Correspondence to Zongfang Wu, Wenhua Zhang or Weixin Huang.

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Supporting information The supporting information is available online at chem.scichina.com and link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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11426_2023_1802_MOESM1_ESM.pdf

Active Copper Structures in ZnO-Cu Interfacial Catalysis: CO2 Hydrogenation to Methanol and Reverse Water-Gas Shift Reactions

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Xiong, W., Wu, Z., Chen, X. et al. Active copper structures in ZnO-Cu interfacial catalysis: CO2 hydrogenation to methanol and reverse water-gas shift reactions. Sci. China Chem. 67, 715–723 (2024). https://doi.org/10.1007/s11426-023-1802-7

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  • DOI: https://doi.org/10.1007/s11426-023-1802-7

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