Surface Reactive Oxygen from Support Corrects the Nominal Supported Metal Size Effect in Controlling the Reactivity for Low-Temperature Ch4/Co2 Reforming

Modulating the metal-support interfacial structure to achieve coke elimination is highly craved for low-temperature CH4/CO2 reforming. Nonetheless, explicit effects of optimizing supported metal size and catalyst support properties remain convoluted and sometimes controversial. Herein, we designed different Pt-CeO2 interfaces by tuning the surface reactive oxygen (SRO) from ceria and in-situ aggregated nanoparticle size developed from single-atom Pt as independent parameters. Intriguingly, the often-emphasized nominal Pt size effect (0.3–10.5 nm) is secondary due to carbon deposition, while the catalyst with high SRO concentrations exhibits outstanding reactivity. In the Pt-Ox-Ce interfacial microstructure, SRO oxidizes the deposited carbon as an oxygen reservoir, renders interfacial Pt atoms remain active from coke, it therefore determines the reactivity with carbon diffusion being rate-determining step. In situ characterizations and theoretical studies explained the reaction mechanism of SRO and carbon elimination. This work provides new insights for the coke-resistant catalyst design and coke elimination mechanism.