Low-Temperature Catalyst Redispersion: A Route to Enhanced Stability of Supported Metal Catalysts?

Aunkon, Rafat H.; Choi, Hyuk; Shimogawa, Ryuichi; Wang, Haodong; Zhang, Lihua; Reece, Christian; Li, Yuanyuan; Kim, Hyun You; Frenkel, Anatoly I.

doi:10.1021/acscatal.5c06004

Low-Temperature Catalyst Redispersion: A Route to Enhanced Stability of Supported Metal Catalysts?

Journal Article · Wed Nov 12 00:00:00 EST 2025 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5c06004· OSTI ID:3007876

Aunkon, Rafat H. ^[1]; ^[2]; Shimogawa, Ryuichi ^[3]; Wang, Haodong ^[1]; ^[4]; ^[5]; ^[6]; ^[7]; ^[8]

Stony Brook Univ., NY (United States)
Chungnam National Univ., Daejeon (Korea, Republic of); Nanyang Technological Univ. (Singapore)
Mitsubishi Chemical Corporation, Yokohama (Japan)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Harvard Univ., Cambridge, MA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Chungnam National Univ., Daejeon (Korea, Republic of)
Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sintering poses a significant challenge to achieving the long-term stability of supported metal catalysts under reaction conditions. Here, in this study, we report a low-temperature catalyst redispersion mechanism, in which platinum single atoms, which aggregate into nanoparticles under Reverse Water Gas Shift (RWGS) conditions at elevated temperatures, fragment into atomically dispersed species upon cooling. Using multimodal operando characterization combined with first-principles theoretical modeling, we track the structural evolution of Pt single atoms supported on ceria nanodomes, deposited either on ceria or ceria–titania mixed oxides. We find that fragmentation is more pronounced when cooling occurs under RWGS conditions compared to CO alone, owing to a synergistic interplay of the effects of H₂, CO₂, and CO. The support architecture has a strong influence on the extent of redispersion: while CO alone induces fragmentation on ceria, interfacial confinement and vacancy pinning at the ceria–titania interface suppress restructuring. In contrast, RWGS conditions overcome these barriers, enabling redispersion across both supports. These findings point toward a pathway for catalyst stabilization via reaction-induced redispersion under mild conditions.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Research Foundation of Korea (NRF); National Science Foundation (NSF); 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:: AC05-00OR22725; SC0012704

OSTI ID:: 3007876

Alternate ID(s):: OSTI ID: 3012576

Report Number(s):: BNL--229305-2026-JAAM

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 22 Vol. 15; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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Low-Temperature Catalyst Redispersion: A Route to Enhanced Stability of Supported Metal Catalysts?

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