TY - JOUR
T1 - Enhancing Metal-Support Interactions of Ru Catalysts via Relaxation of Oxygen Vacancies for Hydrogen Production
AU - Kim, Mansu
AU - Park, Jonghwan
AU - Choi, Hyuk
AU - Kim, Sohui
AU - Jang, Injoon
AU - Kim, Hyun You
AU - Jung, Namgee
AU - Yoo, Sung Jong
AU - Hupp, Joseph T.
AU - Whang, Dongmok
N1 - Publisher Copyright:
© 2025 The Author(s). Advanced Functional Materials published by Wiley-VCH GmbH.
PY - 2026/1/12
Y1 - 2026/1/12
N2 - 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 ZrO2-x, CeO2-x, and ZrCeO2-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-ZrCeO2-x exhibited superior structural stability compared to Ru-ZrO2-x and Ru-CeO2-x, particularly under high-potential sweep (HPS) conditions. The incorporation of Ce into ZrO2-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 ZrCeO2-x as a robust support material for Ru-based catalysts, advancing their potential for durable and efficient energy applications.
AB - 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 ZrO2-x, CeO2-x, and ZrCeO2-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-ZrCeO2-x exhibited superior structural stability compared to Ru-ZrO2-x and Ru-CeO2-x, particularly under high-potential sweep (HPS) conditions. The incorporation of Ce into ZrO2-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 ZrCeO2-x as a robust support material for Ru-based catalysts, advancing their potential for durable and efficient energy applications.
KW - Ru catalyst
KW - ZrCeO support
KW - hydrogen evolution reaction
KW - lattice relaxation
KW - metal-organic framework
KW - metal-support interaction
KW - oxygen vacancies
UR - https://www.scopus.com/pages/publications/105011820599
U2 - 10.1002/adfm.202506866
DO - 10.1002/adfm.202506866
M3 - Article
AN - SCOPUS:105011820599
SN - 1616-301X
VL - 36
JO - Advanced Functional Materials
JF - Advanced Functional Materials
IS - 4
M1 - e06866
ER -
