Superexchange-stabilized long-distance Cu sites in rock-salt-ordered double perovskite oxides for CO2 electromethanation

Jiawei Zhu (), Yu Zhang, Zitao Chen, Zhenbao Zhang, Xuezeng Tian, Minghua Huang, Xuedong Bai, Xue Wang, Yongfa Zhu and Heqing Jiang ()
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Jiawei Zhu: Chinese Academy of Sciences
Yu Zhang: Chinese Academy of Sciences
Zitao Chen: Chinese Academy of Sciences
Zhenbao Zhang: Linyi University
Xuezeng Tian: Chinese Academy of Sciences
Minghua Huang: Ocean University of China
Xuedong Bai: Chinese Academy of Sciences
Xue Wang: City University of Hong Kong
Yongfa Zhu: Tsinghua University
Heqing Jiang: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Cu-oxide-based catalysts are promising for CO2 electroreduction (CO2RR) to CH4, but suffer from inevitable reduction (to metallic Cu) and uncontrollable structural collapse. Here we report Cu-based rock-salt-ordered double perovskite oxides with superexchange-stabilized long-distance Cu sites for efficient and stable CO2-to-CH4 conversion. For the proof-of-concept catalyst of Sr2CuWO6, its corner-linked CuO6 and WO6 octahedral motifs alternate in all three crystallographic dimensions, creating sufficiently long Cu-Cu distances (at least 5.4 Å) and introducing marked superexchange interaction mainly manifested by O-anion-mediated electron transfer (from Cu to W sites). In CO2RR, the Sr2CuWO6 exhibits significant improvements (up to 14.1 folds) in activity and selectivity for CH4, together with well boosted stability, relative to a physical-mixture counterpart of CuO/WO3. Moreover, the Sr2CuWO6 is the most effective Cu-based-perovskite catalyst for CO2 methanation, achieving a remarkable selectivity of 73.1% at 400 mA cm−2 for CH4. Our experiments and theoretical calculations highlight the long Cu-Cu distances promoting *CO hydrogenation and the superexchange interaction stabilizing Cu sites as responsible for the superb performance.

Date: 2024
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DOI: 10.1038/s41467-024-45747-5

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