Developing efficient catalysts for the total oxidation of light alkane at low temperatures is challenging. In this study, superior catalytic performance in the total oxidation of light alkane was achieved by modulating the acidity and redox property of a Pt/CeO2 catalyst through phosphorus modification. Surface modification with phosphorus resulted in electron withdrawal from Pt, leading to platinum species with high valency and the generation of Brönsted acid sites, leading to increased acidity of the Pt/CeO2 catalyst. Consequently, the ability of the Pt/CeO2 catalyst to activate the C-H bond increased with increasing P content in the catalyst owing to the synergistic effect of Ptδ+-(CeO2-POx)δ- dipolar catalytic sites. In contrast, the redox property of the Pt/CeO2 catalyst weakened at first; subsequently, it was partially restored owing to the recovery of a part of the bare ceria surface with increasing P content. The turnover frequency in propane oxidation over the phosphate-modified Pt/CeO2 catalyst with a P/Ce atomic ratio of 0.06 was 10-fold higher than that over the unmodified Pt/CeO2 catalyst at 220 °C. This comprehensive study not only sheds light on the mechanism underlying the surface modification process but also offers a strategy for realizing higher catalytic activity in the total oxidation of light alkanes.
Keywords: C−H bond; phosphorus modification; propane oxidation; redox property; surface acidity.