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

Abstract

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 °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.