Site Diversity and Mechanism of Metal–Exchanged Zeolite Catalyzed Non–Oxidative Propane Dehydrogenation

Yuan, Yong; Zhao, Zhaoqi; Lobo, Raul F.; Xu, Bingjun

doi:10.1002/advs.202207756

Site Diversity and Mechanism of Metal–Exchanged Zeolite Catalyzed Non–Oxidative Propane Dehydrogenation

Journal Article · Thu Mar 09 23:00:00 EST 2023 · Advanced Science

DOI:https://doi.org/10.1002/advs.202207756· OSTI ID:2007300

Yuan, Yong ^[1]; Zhao, Zhaoqi ^[2]; Lobo, Raul F. ^[3]; ^[4]

University of Delaware, Newark, DE (United States); Peking University
Peking University, Beijing (China)
University of Delaware, Newark, DE (United States)
University of Delaware, Newark, DE (United States); Peking University, Beijing (China)

Metal-exchanged zeolites are well-known propane dehydrogenation (PDH) catalysts; however, the structure of the active species remains unresolved. In this review, existing PDH catalysts are first surveyed, and then the current understanding of metal-exchanged zeolite catalysts is described in detail. The case of Ga/H-ZSM-5 is employed to showcase that advances in the understanding of structure–activity relations are often accompanied by technological or conceptional breakthroughs. The understanding of Ga speciation at PDH conditions has evolved owing to the advent of in situ/operando characterizations and to the realization that the local coordination environment of Ga species afforded by the zeolite support has a decisive impact on the active site structure. In situ/operando quantitative characterization of catalysts, rigorous determination of intrinsic reaction rates, and predictive computational modeling are all significant in identifying the most active structure in these complex systems. The reaction mechanism could be both intricately related to and nearly independent of the details of the assumed active structure, as in the two main proposed PDH mechanisms on Ga/H-ZSM-5, that is, the carbenium mechanism and the alkyl mechanism. Perspectives on potential approaches to further elucidate the active structure of metal-exchanged zeolite catalysts and reaction mechanisms are discussed in the final section.

View Accepted Manuscript (DOE)

Research Organization:: RAPID Manufacturing Institute, New York, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Energy Efficiency Office. Advanced Materials & Manufacturing Technologies Office (AMMTO)

Grant/Contract Number:: EE0007888

OSTI ID:: 2007300

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 13 Vol. 10; ISSN 2198-3844

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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