CeO2/Cu2O/Cu Tandem Interfaces for Efficient Water-Gas Shift Reaction Catalysis

Zhengjian Li; Mingzhi Wang; Yanyan Jia; Ruian Du; Tan Li; Yanping Zheng; Mingshu Chen; Yongcai Qiu; Keyou Yan; Wei-Wei Zhao; Pei Wang; Geoffrey I N Waterhouse; Sheng Dai; Yun Zhao; Guangxu Chen

doi:10.1021/acsami.3c06386

CeO₂/Cu₂O/Cu Tandem Interfaces for Efficient Water-Gas Shift Reaction Catalysis

ACS Appl Mater Interfaces. 2023 Jul 5;15(26):31584-31594. doi: 10.1021/acsami.3c06386. Epub 2023 Jun 20.

Authors

Zhengjian Li¹, Mingzhi Wang¹, Yanyan Jia², Ruian Du¹, Tan Li¹, Yanping Zheng³, Mingshu Chen³, Yongcai Qiu¹, Keyou Yan¹, Wei-Wei Zhao⁴, Pei Wang⁵, Geoffrey I N Waterhouse⁶, Sheng Dai², Yun Zhao¹, Guangxu Chen¹

Affiliations

¹ School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou, Guangdong 510006, China.
² Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Centre, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science & Technology, Shanghai 200237, China.
³ State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China.
⁴ State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China.
⁵ College of Science, Huazhong Agricultural University, Wuhan 430074, PR China.
⁶ School of Chemical Sciences, The University of Auckland, Auckland 1142, New Zealand.

PMID: 37339248
DOI: 10.1021/acsami.3c06386

Abstract

Metal-oxide interfaces on Cu-based catalysts play very important roles in the low-temperature water-gas shift reaction (LT-WGSR). However, developing catalysts with abundant, active, and robust Cu-metal oxide interfaces under LT-WGSR conditions remains challenging. Herein, we report the successful development of an inverse copper-ceria catalyst (Cu@CeO₂), which exhibited very high efficiency for the LT-WGSR. At a reaction temperature of 250 °C, the LT-WGSR activity of the Cu@CeO₂ catalyst was about three times higher than that of a pristine Cu catalyst without CeO₂. Comprehensive quasi-in situ structural characterizations indicated that the Cu@CeO₂ catalyst was rich in CeO₂/Cu₂O/Cu tandem interfaces. Reaction kinetics studies and density functional theory (DFT) calculations revealed that the Cu⁺/Cu⁰ interfaces were the active sites for the LT-WGSR, while adjacent CeO₂ nanoparticles play a key role in activating H₂O and stabilizing the Cu⁺/Cu⁰ interfaces. Our study highlights the role of the CeO₂/Cu₂O/Cu tandem interface in regulating catalyst activity and stability, thus contributing to the development of improved Cu-based catalysts for the LT-WGSR.

Keywords: Cu+/Cu0 interface; Cu−CeO2 catalyst; hydrogen production; low-temperature WGS reaction; tandem interface.