Generating active metal/oxide reverse interfaces through coordinated migration of single atoms

Lina Zhang, Shaolong Wan,Congcong Du, Qiang Wan,Hien Pham, Jiafei Zhao,Xingyu Ding, Diye Wei,Wei Zhao, Jiwei Li,Yanping Zheng, Hui Xie, Hua Zhang,Mingshu Chen, Kelvin H. L. Zhang, Shuai Wang,Jingdong Lin, Jianyu Huang,Sen Lin, Yong Wang,Abhaya K. Datye, Ye Wang,Haifeng Xiong

NATURE COMMUNICATIONS(2024)

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摘要
Identification of active sites in catalytic materials is important and helps establish approaches to the precise design of catalysts for achieving high reactivity. Generally, active sites of conventional heterogeneous catalysts can be single atom, nanoparticle or a metal/oxide interface. Herein, we report that metal/oxide reverse interfaces can also be active sites which are created from the coordinated migration of metal and oxide atoms. As an example, a Pd1/CeO2 single-atom catalyst prepared via atom trapping, which is otherwise inactive at 30 degrees C, is able to completely oxidize formaldehyde after steam treatment. The enhanced reactivity is due to the formation of a Ce2O3-Pd nanoparticle domain interface, which is generated by the migration of both Ce and Pd atoms on the atom-trapped Pd1/CeO2 catalyst during steam treatment. We show that the generation of metal oxide-metal interfaces can be achieved in other heterogeneous catalysts due to the coordinated mobility of metal and oxide atoms, demonstrating the formation of a new active interface when using metal single-atom material as catalyst precursor. Steam treatment transforms inactive Pd1/CeO2 catalyst into a highly reactive one by forming a Ce2O3-Pd nanoparticle interface. This domain interface is created by the coordinated migration of Ce and Pd atoms on the atom trapped Pd1/CeO2.
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