Direct OC-CHO coupling towards highly C2+ products selective electroreduction over stable Cu0/Cu2+ interface

Xin Yu Zhang; Zhen Xin Lou; Jiacheng Chen; Yuanwei Liu; Xuefeng Wu; Jia Yue Zhao; Hai Yang Yuan; Minghui Zhu; Sheng Dai; Hai Feng Wang; Chenghua Sun; Peng Fei Liu; Hua Gui Yang

doi:10.1038/s41467-023-43182-6

Direct OC-CHO coupling towards highly C₂₊ products selective electroreduction over stable Cu⁰/Cu²⁺ interface

Nat Commun. 2023 Nov 24;14(1):7681. doi: 10.1038/s41467-023-43182-6.

Authors

Xin Yu Zhang^#¹, Zhen Xin Lou^#¹, Jiacheng Chen², Yuanwei Liu¹, Xuefeng Wu¹, Jia Yue Zhao¹, Hai Yang Yuan³, Minghui Zhu², Sheng Dai⁴, Hai Feng Wang⁵, Chenghua Sun⁶, Peng Fei Liu⁷, Hua Gui Yang⁸

Affiliations

¹ Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
² State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
³ Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China. hyyuan@ecust.edu.cn.
⁴ Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
⁵ Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China.
⁶ Department of Chemistry and Biotechnology, and Center for Translational Atomaterials, Swinburne University of Technology, Hawthorn, VIC, 3122, Australia.
⁷ Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China. pfliu@ecust.edu.cn.
⁸ Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, School of Materials Science and Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai, 200237, China. hgyang@ecust.edu.cn.

^# Contributed equally.

Abstract

Electroreduction of CO₂ to valuable multicarbon (C₂₊) products is a highly attractive way to utilize and divert emitted CO₂. However, a major fraction of C₂₊ selectivity is confined to less than 90% by the difficulty of coupling C-C bonds efficiently. Herein, we identify the stable Cu⁰/Cu²⁺ interfaces derived from copper phosphate-based (CuPO) electrocatalysts, which can facilitate C₂₊ production with a low-energy pathway of OC-CHO coupling verified by in situ spectra studies and theoretical calculations. The CuPO precatalyst shows a high Faradaic efficiency (FE) of 69.7% towards C₂H₄ in an H-cell, and exhibits a significant FE_C2+ of 90.9% under industrially relevant current density (j = -350 mA cm^-2) in a flow cell configuration. The stable Cu⁰/Cu²⁺ interface breaks new ground for the structural design of electrocatalysts and the construction of synergistic active sites to improve the activity and selectivity of valuable C₂₊ products.