Abstract
Up to now, methane combustion catalysts generally suffer from issues such as poor reaction stability and susceptibility to sulfur poisoning, which have become the key factors restricting their application, so it is necessary to construct catalysts with excellent chemical stability of the active center and strong sulfur resistance. Here, we showed the crystal phase-modulated state of PtOx nanoparticles (PtOx NPs) on TiO2 and investigated their effects on the reactivity of methane catalytic combustion and anti-SO2 poisoning properties. It was found that Pt/r-TiO2 showed superior activity, stability, and resistance to SO2 poisoning. Transmission electron microscope (TEM) images showed that the PtOx NPs on the surface of r-TiO2 were much more stable than a-TiO2 for the reason that the Ostwald ripening of PtOx NPs on a-TiO2 was facilitated due to the strong metal-support interaction (MSI) between PtOx NPs and TiO2 and the low migration energy of the PtOx NPs on TiO2, while they were moderate of Pt/r-TiO2, and then the active sites were stabilized during methane combustion. The activity was controlled by the size and electronic structure of PtOx NPs, which were stable on the surface of r-TiO2 with a higher Pt4+ content, and the density functional theory (DFT) calculations further revealed the role of r-TiO2 in increasing the quantities of surface oxygen vacancies. Moreover, the SO2 tolerance of Pt/r-TiO2 was also the best among all kinds of Pt-based catalysts prepared, which was attributed to the minimal adsorption energy (Ead) of SO2 on r-TiO2, and the absence of sulfate and sulfite deposition on the Pt/r-TiO2 catalyst confirmed by TGA and in-situ DRIFTS studies on SO2 adsorption. In this research, the anti-SO2 poisoning and reaction stability were realized by adjusting the interaction between SO2, active components, and supports, which provided a new insight for the design of stable Pt-based SO2-resistant catalysts.
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