Zinc Migration Mediates Isolated [PtFe3] in Zeolite for Propane Dehydrogenation

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-02-07 DOI:10.1021/acscatal.4c05199

Mingrui Xu, Bofeng Zhang, Rongrong Zhang, Liming Xia, Guozhu Liu

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Abstract

Structural transformation under in situ reaction conditions plays a vital role in heterogeneous catalytic performance, especially caused by metal migration. However, the migration of active components often leads to irreversible structural disruption at high temperatures, which could be associated with the deactivation of catalysts. Here, we report a low-melting-point Zn migration-mediated strategy to synthesize ultrastable isolated PtFe₃ sites anchored in MFI zeolite for propane direct dehydrogenation. The optimized catalyst exhibited a superior specific activity of 36.5 mol C₃H₆ mol_Pt^–1 s^–1 with propylene selectivity above 99% at 550 °C. Moreover, the dehydrogenation activity remained stable after over 400 h on stream with a low deactivation rate constant of 0.001 h^–1 under industrial conditions at 580 °C. In situ characterizations demonstrated that Fe³⁺ species were conducive to the rearrangement in the electronic configuration of the unoccupied 5d states of Pt atoms to form electron-deficient Pt sites. This strategy could afford insights into the dynamic evolution of catalyst preparation in heterogeneous processes.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.