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

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

doi:10.1002/adfm.202506866

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

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

Department of Advanced Materials Science and Engineering

Northwestern University
Sungkyunkwan University
Chungnam National University
Chungbuk National University
Korea Institute of Science and Technology
University of Science and Technology UST

Research output: Contribution to journal › Article › peer-review

11 Scopus citations

Abstract

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.

Original language	English
Article number	e06866
Journal	Advanced Functional Materials
Volume	36
Issue number	4
DOIs	https://doi.org/10.1002/adfm.202506866
State	Published - 12 Jan 2026

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

Ru catalyst
ZrCeO support
hydrogen evolution reaction
lattice relaxation
metal-organic framework
metal-support interaction
oxygen vacancies

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10.1002/adfm.202506866

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title = "Enhancing Metal-Support Interactions of Ru Catalysts via Relaxation of Oxygen Vacancies for Hydrogen Production",

abstract = "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.",

keywords = "Ru catalyst, ZrCeO support, hydrogen evolution reaction, lattice relaxation, metal-organic framework, metal-support interaction, oxygen vacancies",

author = "Mansu Kim and Jonghwan Park and Hyuk Choi and Sohui Kim and Injoon Jang and Kim, \{Hyun You\} and Namgee Jung and Yoo, \{Sung Jong\} and Hupp, \{Joseph T.\} and Dongmok Whang",

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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

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

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DO - 10.1002/adfm.202506866

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SN - 1616-301X

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IS - 4

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ER -

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

Abstract

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Keywords

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