Ce-induced synergistic effect in exsolved perovskite catalyst for highly efficient and robust methane dry reforming

Chencun Hao, Zhiyu Qu, Louise R. Smith, Nicholas F. Dummer, Haifeng Qi, Thomas J. A. Slater, Zhiping Zhu, Riguang Zhang (), Zhao Sun (), Zhiqiang Sun () and Graham J. Hutchings ()
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Chencun Hao: Central South University, Hunan Engineering Research Center of Clean and Low-Carbon Energy Technology, School of Energy Science and Engineering
Zhiyu Qu: Taiyuan University of Technology, State Key Laboratory of Clean and Efficient Coal Utilization, College of Chemical Engineering and Technology
Louise R. Smith: Cardiff University, Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry
Nicholas F. Dummer: Cardiff University, Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry
Haifeng Qi: Cardiff University, Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry
Thomas J. A. Slater: Cardiff University, Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry
Zhiping Zhu: Chinese Academy of Sciences, State Key Laboratory of Coal Conversion, Institute of Engineering Thermophysics
Riguang Zhang: Taiyuan University of Technology, State Key Laboratory of Clean and Efficient Coal Utilization, College of Chemical Engineering and Technology
Zhao Sun: Central South University, Hunan Engineering Research Center of Clean and Low-Carbon Energy Technology, School of Energy Science and Engineering
Zhiqiang Sun: Central South University, Hunan Engineering Research Center of Clean and Low-Carbon Energy Technology, School of Energy Science and Engineering
Graham J. Hutchings: Cardiff University, Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Cardiff Catalysis Institute, School of Chemistry

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Dry reforming of methane is an effective approach to convert two major greenhouse gases, methane and carbon dioxide, into high-value syngas, used as a feedstock for bulk and fine chemical synthesis. However, catalyst deactivation and carbon deposition under harsh conditions hinder its industrialization process. Herein, we present a Ce-modified and Ni-exsolved perovskite catalyst, 0.2Ce-La0.97Ni0.4Cr0.6O3, for achieving highly efficient and robust CH4-CO2 reforming with CH4 and CO2 conversions of 87.4% and 92.9% at 800 °C, respectively. Moreover, this unique catalyst exhibits remarkable stability, maintaining its superior activity over 800 h. Characterization and density functional theory reveal that two Ce species are present: surface oxygen vacancy-moderate CeO2-x (Cesurf) and bulk lattice Ce (Cebulk). These play a specific role in methane dry reforming, where the Cesurf promotes CO2 adsorption and hinders carbon deposition, while Cebulk induces lattice strain and Ni exsolution, key factors contributing to the high activity and stability.

Date: 2025
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DOI: 10.1038/s41467-025-65619-w

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