Enhancing Metal‐Support Interactions of Ru Catalysts via Relaxation of Oxygen Vacancies for Hydrogen Production

Kim, Mansu; Park, Jonghwan; Choi, Hyuk; Kim, Sohui; Jang, Injoon; Kim, Hyun You; Jung, Namgee; Yoo, Sung Jong; Hupp, Joseph T.; Whang, Dongmok

doi:10.1002/adfm.202506866

Enhancing Metal‐Support Interactions of Ru Catalysts via Relaxation of Oxygen Vacancies for Hydrogen Production

Journal Article · Thu Jul 24 00:00:00 UTC 2025 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202506866· OSTI ID:2901173

^[1]; Park, Jonghwan ^[2]; Choi, Hyuk ^[3]; Kim, Sohui ^[2]; Jang, Injoon ^[4]; Kim, Hyun You ^[3]; Jung, Namgee ^[3]; Yoo, Sung Jong ^[5]; Hupp, Joseph T. ^[6]; Whang, Dongmok ^[2]

Northwestern Univ., Evanston, IL (United States); Sungkyunkwan Univ., Suwon (Republic of Korea)
Sungkyunkwan Univ., Suwon (Republic of Korea)
Chungnam National Univ., Daejeon (Korea, Republic of)
Chungbuk National Univ. (Korea, Republic of)
Korea Institute of Science and Technology (KIST) (Korea, Republic of); Univ. of Science and Technology (UST), Daejeon (Korea, Republic of)
Northwestern Univ., Evanston, IL (United States)

The stability of Ru-based catalysts under harsh electrochemical conditions is a critical challenge limiting their practical application in energy conversion systems. In this study, Ru catalysts supported on ZrO_2-x, CeO_2-x, and ZrCeO_2-x are synthesized via pyrolysis of metal-organic frameworks (MOFs) and systematically evaluated to elucidate the role of support interactions on catalytic performance and durability. Advanced characterization techniques, including HR-TEM, XRD, XPS, and EXAFS, revealed that Ru-ZrCeO_2-x exhibited superior structural stability compared to Ru-ZrO_2-x and Ru-CeO_2-x, particularly under high-potential sweep (HPS) conditions. The incorporation of Ce into ZrO_2-x is shown to stabilize oxygen vacancies and enhance the interaction between Ru catalyst and the support, thereby mitigating catalyst degradation. Density functional theory (DFT) calculations further confirmed that Ce doping decreases formation energy of the oxygen vacancy, providing a thermodynamically favorable environment for Ru stabilization. This work demonstrates the promise of ZrCeO_2-x as a robust support material for Ru-based catalysts, advancing their potential for durable and efficient energy applications.

View Accepted Manuscript (DOE)

Research Organization:: Chungbuk National Univ., Choengju (Korea, Republic of); Chungnam National Univ., Daejeon (Korea, Republic of); Korea Institute of Science and Technology (KIST), Bucheon (Korea, Republic of); Northwestern Univ., Evanston, IL (United States); Sungkyunkwan Univ., Suwon (Korea, Republic of)

Sponsoring Organization:: National Research Foundation of Korea; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-06CH11357; FG02-87ER13808

OSTI ID:: 2901173

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 4 Vol. 36; ISSN 1616-3028; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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