Abstract
Herein, ZrOSO4 nanoflowers with high sulfates content and the coexistence of (SO3)ad and SO42- species has been developed as the support of Pt-based catalysts for propane combustion. Compared with the Pt catalysts supported on conventional sulfated-ZrO2 and ZrO2, the Pt/ZrOSO4 gives the highest specific reaction rate of 355 μmol gPt−1 s−1 at 190 °C, the TOF value on Pt/ZrOSO4 is 2 times of that on Pt/sulfated-ZrO2 and 7 times of that on Pt/ZrO2. Differentfrom that only SO42- on the Pt/sulfated-ZrO2, there are two sulfate species on the Pt/ZrOSO4, conventional SO42- and (SO3)ad. The presence of sulfates not only leads to the formation of Brønsted acid sites and promotes the propane adsorption, but also significantly affects the chemical states of Pt species. The interaction between Pt and SO42- results in the formation of reactive Pt0 species, which facilitates the CC bond activation, and the Pt-(SO3)ad electronic interaction is beneficial for the generation of the metastable Pt+, which further promotes propanecombustion via heterolytic CH bond activation. Moreover, the Pt/ZrOSO4 also can provide active oxygen species with enhanced oxygen mobility and reactivity due to the presence of Pt-O-SO3 species, which can accelerate the oxidation of reaction intermediates. This workcontributes to in-depth insight into the role of different sulfate species for propane combustion over Pt-based catalysts.
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