Migration and aggregation of Pt atoms on metal oxide-supported ceria nanodomes control reverse water gas shift reaction activity

Wang, Haodong; Shimogawa, Ryuichi; Zhang, Lihua; Ma, Lu; Ehrlich, Steven N.; Marinkovic, Nebojsa; Li, Yuanyuan; Frenkel, Anatoly I.

doi:10.1038/s42004-023-01064-4

Migration and aggregation of Pt atoms on metal oxide-supported ceria nanodomes control reverse water gas shift reaction activity

Journal Article · Tue Dec 05 00:00:00 EST 2023 · Communications Chemistry

DOI:https://doi.org/10.1038/s42004-023-01064-4· OSTI ID:2228552

Wang, Haodong; Shimogawa, Ryuichi; Zhang, Lihua; Ma, Lu; Ehrlich, Steven N.; ; ;

Abstract

Single-atom catalysts (SACs) are particularly sensitive to external conditions, complicating the identification of catalytically active species and active sites under in situ or operando conditions. We developed a methodology for tracing the structural evolution of SACs to nanoparticles, identifying the active species and their link to the catalytic activity for the reverse water gas shift (RWGS) reaction. The new method is illustrated by studying structure-activity relationships in two materials containing Pt SACs on ceria nanodomes, supported on either ceria or titania. These materials exhibited distinctly different activities for CO production. Multimodal operando characterization attributed the enhanced activity of the titania-supported catalysts at temperatures below 320 ˚C to the formation of unique Pt sites at the ceria-titania interface capable of forming Pt nanoparticles, the active species for the RWGS reaction. Migration of Pt nanoparticles to titania support was found to be responsible for the deactivation of titania-supported catalysts at elevated temperatures. Tracking the migration of Pt atoms provides a new opportunity to investigate the activation and deactivation of Pt SACs for the RWGS reaction.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704; SC0022199

OSTI ID:: 2228552

Alternate ID(s):: OSTI ID: 2267557

Report Number(s):: BNL--225114-2023-JAAM; 264; PII: 1064

Journal Information:: Communications Chemistry, Journal Name: Communications Chemistry Journal Issue: 1 Vol. 6; ISSN 2399-3669

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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