▎ 摘　　要

Constructing catalysts with electronic metal-support interaction (EMSI) is promising for catalytic reactions. Herein, graphene-supported positively charged (Pt2+/Pt4+) atomically dispersed Pt catalysts (AD-Pt-G) with PtxC3 (x = 1, 2, and 4)-based EMSI coordination structures are achieved for boosting the catalytic ozonation for odorous CH3SH removal. A CH3SH removal efficiency of 91.5% can be obtained during catalytic ozonation using optimum 0.5AD-Pt-G within 12 h under a gas hourly space velocity of 60,000 mL h(-1) g(-1), whereas that of pure graphene is 40.4%. Proton transfer reaction time-of-flight mass spectrometry, in situ diffuse reflectance infrared Fourier transform spectroscopy/Raman, and electron spin resonance verify that the PtxC3 coordination structure with atomic Pt2+ sites on AD-Pt-G can activate O-2 to generate peroxide species (*O-2) for partial oxidation of CH3SH during the adsorption period and trigger O-3 into surface atomic oxygen (*Oad), *O-2, and superoxide radicals (center dot O-2(-)) to accomplish a stable, high-efficiency, and deeper oxidation of CH3SH during the catalytic ozonation stage. Moreover, the results of XPS and DFT calculation imply the occurrence of Pt2+ -> Pt4+ -> Pt2+ recirculation on PtxC(3) for ADPt-G to maintain the continuous catalytic ozonation for 12 h, i.e., Pt2+ species devote electrons in 5d-orbitals to activate O-3, while Pt4+ species can be reduced back to Pt2+ via capturing electrons from CH3SH. This study can provide novel insights into the development of atomically dispersed Pt catalysts with a strong EMSI effect to realize excellent catalytic ozonation for air purification.