Looping metal-support interaction in heterogeneous catalysts during redox reactions.

Pan, Yue; Zhen, Shiyu; Liu, Xiaozhi; Ge, Mengshu; Zhao, Jianxiong; Gu, Lin; Zhou, Dan; Zhang, Liang et al. · Nat Commun · 2025

basic_science · Level V

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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-Fe<sub>3</sub>O<sub>4</sub> catalysts during the hydrogen oxidation reaction. At the NiFe-Fe<sub>3</sub>O<sub>4</sub> 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 Fe<sub>3</sub>O<sub>4</sub> 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 Fe<sub>3</sub>O<sub>4</sub> 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.