Looping metal-support interaction in heterogeneous catalysts during redox reactions

Yue Pan, Shiyu Zhen, Xiaozhi Liu, Mengshu Ge, Jianxiong Zhao, Lin Gu, Dan Zhou (), Liang Zhang () and Dong Su ()
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Yue Pan: Chinese Academy of Sciences
Shiyu Zhen: Tsinghua University
Xiaozhi Liu: Chinese Academy of Sciences
Mengshu Ge: Chinese Academy of Sciences
Jianxiong Zhao: Chinese Academy of Sciences
Lin Gu: Tsinghua University
Dan Zhou: DENSsolutions B.V.
Liang Zhang: Tsinghua University
Dong Su: Chinese Academy of Sciences

Nature Communications, 2025, vol. 16, issue 1, 1-9

Abstract: Abstract Metal-support interfaces fundamentally govern the catalytic performance of heterogeneous systems through complex interactions. Here, utilizing operando transmission electron microscopy, we uncover a looping metal-support interaction in NiFe-Fe3O4 catalysts during the hydrogen oxidation reaction. At the NiFe-Fe3O4 interfaces, lattice oxygens react with NiFe-activated H atoms, gradually sacrificing themselves and resulting in dynamically migrating interfaces. Meanwhile, reduced iron atoms migrate to the {111} surface of Fe3O4 support and react with oxygen molecules. Consequently, the hydrogen oxidation reaction separates spatially on a single nanoparticle and is intrinsically coupled with the redox reaction of the Fe3O4 support through the dynamic migration of metal-support interfaces. Our work provides previously unidentified mechanistic insight into metal-support interactions and underscores the transformative potential of operando methodologies for studying atomic-scale dynamics.

Date: 2025
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DOI: 10.1038/s41467-025-63646-1

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