Spontaneous Nano‐ZrO <sub>2</sub> Exsolution from Ni‐Zr‐O Mixed Oxides Enables Facile Fabrication of ZrO <sub>2</sub> /Ni Inverse Catalysts for Efficient CO <sub>x</sub> Methanation

X Xin Tang Y Yuanchang Wang J Jinrong Zhang (State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang 310014 China) C Cheng Yu (Department of Spinal Surgery, Zhujiang Hospital, Southern Medical University) M Mengyao Cheng (State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang 310014 China) S Shiqing Yang (State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang 310014 China) X Xuguang Yang L Liangwei Liu L Lili Han (State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter) Y Yao Xu (Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering) C Chuqiao Song L Lili Lin (State Key Laboratory of Green Chemical Synthesis and Conversion, College of Chemical Engineering)

Abstract

Abstract Ni‐based inverse catalysts with nano‐oxide dispersed on metallic substrates have emerged as promising candidates for low‐temperature CO 2 methanation, but it remains challenging in facile synthesis of well‐dispersed oxide‐metal interactions. Herein, a spontaneous oxide exsolution strategy for the fabrication of Ni‐based inverse catalyst via monodispersed Zr species of Ni‐Zr‐O mixed oxide is demonstrated, where precisely tailored calcination and reduction of the mixed oxide enable in situ nano‐ZrO 2 segregation on the metallic Ni matrix. The formation evolution of inverse configuration is elucidated through comprehensive ex situ/in situ characterizations. X‐ray photoelectron spectroscopy reveals the electron transfer between the exsolved ZrO 2 and the Ni matrix, indicating the presence of metal‐oxide interactions. The prepared ZrO 2 /Ni inverse catalyst achieves ∼90% CO 2 conversion and &gt;99% CH 4 selectivity at low‐temperature of 200 °C, and also demonstrates excellent catalytic performance and dynamic operational stability in complex CO x hydrogenation reactions, validating its industrial applicability under realistic syngas‐equivalent feedstock conditions.

Article Details

Volume / Issue Vol. 64, Issue 36
Published September 01, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (12)

X

Xin Tang

Y

Yuanchang Wang

J

Jinrong Zhang

State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang 310014 China

C

Cheng Yu

Department of Spinal Surgery, Zhujiang Hospital, Southern Medical University

M

Mengyao Cheng

State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang 310014 China

S

Shiqing Yang

State Key Laboratory of Green Chemical Synthesis and Conversion Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering Zhejiang University of Technology Hangzhou Zhejiang 310014 China

X

Xuguang Yang

L

Liangwei Liu

L

Lili Han

State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter

Y

Yao Xu

Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering

C

Chuqiao Song

L

Lili Lin

State Key Laboratory of Green Chemical Synthesis and Conversion, College of Chemical Engineering