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Electronic perturbation-promoted interfacial pathway for facile C–H dissociation

CHINESE JOURNAL OF CATALYSIS [2024]
Zhe Wang, Chunpeng Wang, Bing Lu, Zhirong Chen, Yong Wang, Shanjun Mao
ABSTRACT

Interface has often played significant role in the behavior of metal-based catalysts during various heterogeneous reactions. Herein, we reported a novel interfacial pathway for propane dehydrogenation on Pt-GaO x dual sites. The active ensemble, composing Pt particles and Ga 2 O 3 clusters, facilitates the facile dissociation of C–H bonds (energy barrier < 0.30 eV) through H-abstraction by O sites, coupled with alkyl stabilization on the Pt surface. Notably, the electronic perturbation of the Pt slab induces higher-lying O 2 p states at the interface, accompanied by a substantial density of states around fermi level. This is in stark contrast to the O species present in Ga 2 O 3 crystals or clusters alone, leading to an exceptionally strong affinity for H and a robust ability for C–H scission. The Pt/Ga-Al 2 O 3 catalysts prepared with Pt nanoparticles decorated by Ga oxide exhibit superior performance compared to Pt/Al 2 O 3 and PtSn/Al 2 O 3 catalysts. This insight into interfacial catalysis contributes to a broader understanding of the origin of the high catalytic efficiency observed in metal-based catalysts.

MATERIALS

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