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Valence restrictive metal-support interaction for boosting catalytic activity of Rh/CeO2 in CO2 hydrogenation

Author

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  • Ze-Kai Yu

    (East China University of Science and Technology)

  • Mingxiang Jiang

    (East China University of Science and Technology)

  • Sheng Dai

    (East China University of Science and Technology)

  • Wangcheng Zhan

    (East China University of Science and Technology)

  • Zhi-Qiang Wang

    (East China University of Science and Technology)

  • Xue-Qing Gong

    (Shanghai Jiao Tong University)

Abstract

Metal-support interactions (MSI) profoundly modulate the catalytic properties of supported nanometal catalysts. However, a comprehensive understanding of their underlying mechanisms largely remains elusive. In this work, we propose a novel valence restrictive metal-support interaction (VR-MSI) through systematic theoretical and experimental studies of the various Rh-modified CeO2(111) surfaces. It reveals that small Rh clusters are oxidized by the CeO2 support and constantly maintain the +2 valence state, thus establishing a clear correlation between their sizes and the electronic properties for each Rh atom. The VR-MSI effect can therefore favor the adsorptions of negatively charged species at small supported Rh clusters through local electrostatic interactions, and for CO2 hydrogenation reactions, the occurrence of active hydride species (H-) can be effectively promoted by the supported Rh nanocluster toward highly selective and active CO2 hydrogenation to CH4. This discovery broadens our understanding of the MSI effect and the mechanism of selective hydrogenation in heterogeneous catalysis, offering new insights into the rational design of advanced hydrogenation catalysts.

Suggested Citation

  • Ze-Kai Yu & Mingxiang Jiang & Sheng Dai & Wangcheng Zhan & Zhi-Qiang Wang & Xue-Qing Gong, 2025. "Valence restrictive metal-support interaction for boosting catalytic activity of Rh/CeO2 in CO2 hydrogenation," Nature Communications, Nature, vol. 16(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-64140-4
    DOI: 10.1038/s41467-025-64140-4
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    References listed on IDEAS

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    1. Peng Jiang & Ludan Zhang & Xiaolong Liu & Chenliang Ye & Peng Zhu & Ting Tan & Dingsheng Wang & Yuguang Wang, 2024. "Tuning oxidant and antioxidant activities of ceria by anchoring copper single-site for antibacterial application," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    2. Jian Zhang & Dezhi Zhu & Jianfeng Yan & Chang-An Wang, 2021. "Strong metal-support interactions induced by an ultrafast laser," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
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