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

Ye, Runping; Ma, Lixuan; Mao, Jianing; Wang, Xinyao; Hong, Xiaoling; Gallo, Alessandro; Ma, Yanfu; Luo, Wenhao; Wang, Baojun; Zhang, Riguang; Duyar, Melis Seher; Jiang, Zheng; Liu, Jian

doi:10.1038/s41467-024-46513-3

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

Journal Article · 08 March 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-46513-3 · OSTI ID:2405194

^[1]; Ma, Lixuan ^[2]; Mao, Jianing ^[3]; Wang, Xinyao ^[4]; Hong, Xiaoling ^[4];

^[5]; Ma, Yanfu ^[4]; Luo, Wenhao ^[6]; Wang, Baojun ^[2];

^[2];

^[7];

^[8];

^[9]

Nanchang University (China). Institute of Applied Chemistry; SLAC
Taiyuan University of Technology (China)
Chinese Academy of Sciences (CAS), Shanghai (China). Shanghai Institute of Applied Physics; University of Chinese Academy of Sciences, Beijing (China)
Chinese Academy of Sciences (CAS), Dalian (China). Dalian Institute of Chemical Physics
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
Inner Mongolia University, Hohhot (China)
Univ. of Surrey, Guildford (United Kingdom). DICP-Surrey Joint Centre for Future Materials
Univ. of Science and Technology of China, Hefei (China). National Synchrotron Radiation Laboratory (NSRL)
Chinese Academy of Sciences (CAS), Dalian (China). Dalian Institute of Chemical Physics; Inner Mongolia University, Hohhot (China); Univ. of Surrey, Guildford (United Kingdom). DICP-Surrey Joint Centre for Future Materials

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·kg_cat^-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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Key R&D Program of China; National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 2405194

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Heterogeneous catalysis
metal-organic frameworks
renewable energy
surface chemistry

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

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