Regulating the Electronic Metal–Support Interaction of Single-Atom Ruthenium Catalysts for Boosting Chlorobenzene Oxidation

Abstract

Developing highly active single-atom catalysts (SACs) with excellent chlorine resistance for efficient oxidation of harmful chlorinated volatile organic compounds (CVOCs) is a great challenge. Tuning the electronic metal–support interaction (EMSI) is viable for promoting catalytic performances of SACs. Herein, an effective strategy of modulating the EMSI in Ru₁/CeO₂ SACs by thermal treatment control is proposed, which distinctly enhances the activities of the catalyst for chlorobenzene (CB) oxidation and chlorine conversion, accomplishing total CB degradation at nearly 260 °C. Detailed characterization and theoretical calculations reveal that the EMSI induces electron transfer from Ru to CeO₂, optimizing the coordination and electronic structure of single-atom Ru and accordingly facilitating the adsorption and activation of CB. Moreover, the surface lattice oxygen (O_latt) at the Ru–O–Ce interface is demonstrated as the critical reactive oxygen species, the mobility and reactivity of which are also prompted by the EMSI, leading to the boosted conversion of reaction intermediates. This work sheds light on the effect of EMSI regulation on CVOC catalytic oxidation and provides guidance on fabricating high-efficiency SACs for environmental catalysis.