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Modulating the active sites in atomic level is very meaningful to optimize catalyst performance but still very challenge. Herein, Pt catalysts loaded on different supports (ZSM-5, Al 2 O 3 , ZrO 2 , CeO 2) were sulfate modified by in situ pyrolysis of (NH 4) 2 SO 4 mixed with Pt catalyst. Sulfate remarkably improves these catalyst activities for propane combustion, particularly for the sulfate modified Pt/ZSM-5 catalyst with the highest activity among them. Through controlling the amount of (NH 4) 2 SO 4 used and the loading of Pt, Pt/S atomic ratio in the sulfate modified Pt/ZSM-5 catalyst was successfully regulated. Pt/S atomic ratio significantly affects the electron transfer from Pt species to sulfate and also their interaction strength, which is decisive to the synergetic catalysis of sulfate and Pt species. The 5S-2Pt/ZSM-5 with Pt/S atomic ratio of 0.5 shows a moderate strength of sulfate and Pt species interaction, which is responsible for its highest reaction rate of 86.5 μmol·g Pt −1·s−1 at 200 °C. [Display omitted] • Pt based catalysts were modified with sulfate species by in situ pyrolysis of (NH 4) 2 SO 4. • Pt/S atomic ratio was successfully regulated to optimize catalytic activity for propane oxidation. • The synergy catalysis of sulfate and Pt species for propane oxidation is affected by their interaction strength. • Moderately strong interaction between sulfate and Pt species achieves the highest activity. [ABSTRACT FROM AUTHOR]