Strategies for regeneration of Pt-alloy catalysts supported on silica for propane dehydrogenation

Alcala, Ryan; Dean, David P.; Chavan, Isha; Chang, Che-Wei; Burnside, Brandon; Pham, Hien N.; Peterson, Eric; Miller, Jeffrey T.; Datye, Abhaya K.

doi:10.1016/j.apcata.2023.119157

Strategies for regeneration of Pt-alloy catalysts supported on silica for propane dehydrogenation

Journal Article · Wed Mar 22 00:00:00 EDT 2023 · Applied Catalysis. A, General

DOI:https://doi.org/10.1016/j.apcata.2023.119157· OSTI ID:2423624

^[1]; Dean, David P. ^[2]; Chavan, Isha ^[2]; Chang, Che-Wei ^[2]; Burnside, Brandon ^[1]; Pham, Hien N. ^[1]; Peterson, Eric ^[1]; Miller, Jeffrey T. ^[2]; Datye, Abhaya K. ^[1]

Univ. of New Mexico, Albuquerque, NM (United States)
Purdue Univ., West Lafayette, IN (United States)

Catalyst stability, resistance to deactivation, and regeneration remain a challenge for high temperature reaction processes. For Pt alloys used in propane dehydrogenation (PDH), the primary pathways of catalyst deactivation include coke formation and metal nanoparticle sintering over time. Recent work shows that silica-supported catalysts provide excellent selectivity for this reaction, but the regenerability of silica-supported catalysts has not been established. In this work, we study a series of Pt alloys, including PtMn, PtZn, and PtSn, for the PDH reaction at 550 °C and 600 °C, and we subject the catalysts to regeneration over multiple cycles. While oxidation in air restores the reactivity completely with minimal catalyst sintering, it is surprising to find that these catalysts can also be regenerated in pure hydrogen. Here we explore the types of coke formed on these catalysts using in situ temperature programmed oxidation (TPO). Two types of coke are found: one on the metallic NP surface, and a second on the silica support. Our work shows that treatment in hydrogen causes redistribution of the coke between the metal and support, which can restore most catalytic activity lost during a reaction run. Finally, periodic introduction of H₂ during a reaction cycle may constitute an unexplored strategy for extending the lifetime of PDH catalysts.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 2423624

Alternate ID(s):: OSTI ID: 1968523

Journal Information:: Applied Catalysis. A, General, Journal Name: Applied Catalysis. A, General Vol. 658; ISSN 0926-860X

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Catalyst stability
H2
Propane dehydrogenation
Pt-alloys
Regeneration
Silica
regeneration

Strategies for regeneration of Pt-alloy catalysts supported on silica for propane dehydrogenation

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