A Ce-CuZn catalyst with abundant Cu/Zn-OV-Ce active sites for CO2 hydrogenation to methanol

Runping Ye, Lixuan Ma, Jianing Mao, Xinyao Wang, Xiaoling Hong, Alessandro Gallo, Yanfu Ma, Wenhao Luo, Baojun Wang, Riguang Zhang (), Melis Seher Duyar (), Zheng Jiang () and Jian Liu ()
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Runping Ye: Nanchang University
Lixuan Ma: Taiyuan University of Technology
Jianing Mao: Chinese Academy of Sciences
Xinyao Wang: Chinese Academy of Sciences
Xiaoling Hong: Chinese Academy of Sciences
Alessandro Gallo: SLAC National Accelerator Laboratory, 2575 Sand Hill Road
Yanfu Ma: Chinese Academy of Sciences
Wenhao Luo: Inner Mongolia University
Baojun Wang: Taiyuan University of Technology
Riguang Zhang: Taiyuan University of Technology
Melis Seher Duyar: Guilford
Zheng Jiang: University of Science and Technology of China
Jian Liu: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract CO2 hydrogenation to chemicals and fuels is a significant approach for achieving carbon neutrality. It is essential to rationally design the chemical structure and catalytic active sites towards the development of efficient catalysts. Here we show a Ce-CuZn catalyst with enriched Cu/Zn-OV-Ce active sites fabricated through the atomic-level substitution of Cu and Zn into Ce-MOF precursor. The Ce-CuZn catalyst exhibits a high methanol selectivity of 71.1% and a space-time yield of methanol up to 400.3 g·kgcat−1·h−1 with excellent stability for 170 h at 260 °C, comparable to that of the state-of-the-art CuZnAl catalysts. Controlled experiments and DFT calculations confirm that the incorporation of Cu and Zn into CeO2 with abundant oxygen vacancies can facilitate H2 dissociation energetically and thus improve CO2 hydrogenation over the Ce-CuZn catalyst via formate intermediates. This work offers an atomic-level design strategy for constructing efficient multi-metal catalysts for methanol synthesis through precise control of active sites.

Date: 2024
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DOI: 10.1038/s41467-024-46513-3

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