Retained Oxygen Regulation in Oxide‐Derived Copper for Promoted CO <sub>2</sub> Electroreduction Toward Multicarbon Products

H Huan Wang H Hai Xiang Yang (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) Y Yi Ning Xu (Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China) H Huai Qin Fu (School of Environment and Science, Gold Coast Campus) X Xin Yan Li (Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China) J Jing Jing He (National Enterprise Technology Center Inner Mongolia Erdos Electric Power and Metallurgy Group Company Limited Ordos Inner Mongolia 016064 China) Q Qiang Niu J Jia Chen Wu (Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China) H Hai Yang Yuan (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) P Peng Fei Liu (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) H Hua Gui Yang (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)

Abstract

Abstract Electrochemical CO 2 reduction to multicarbon products provides an attractive route to store intermittent renewable electricity as high value‐added chemicals. Oxide‐derived Cu (OD‐Cu) has been widely investigated for its tunable selectivity toward multicarbon (C 2+ ) products; however, it still remains a challenge to understand and regulate the retained oxygen of OD‐Cu in the complex reconstruction process. In this work, we investigate thickness determined residual oxygen in OD‐Cu, using CuO nanosheets as prototype precatalysts. When the thickness of CuO precatalyst decreased to 1.6 nm, the enhancement of the ability to retain oxygen are achieved, leading to selective C 2+ production with Faradaic efficiency of around 80% over a wide current density range of 300–700 mA cm −2 with a peak value of 84.6% at 700 mA cm −2 . Long‐time molecular dynamics simulations reveal the enhanced stability of Cu–CuO structure with the layers of removed oxygen increased, favoring *CHO formation and *OC‐CHO coupling toward C 2+ products; structural characterizations and electrochemical results further demonstrate the reconstructed stacked nanosheets with high oxygen retention capacity and easily reoxidized metallic Cu sites. This work underscores the crucial role of the retained oxygen for the OD‐Cu performance and provides insights into designing OD‐Cu with oxygen retention to enhance C 2+ products formation.

Article Details

Volume / Issue Vol. 64, Issue 25
Published June 17, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (11)

H

Huan Wang

H

Hai Xiang Yang

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

Y

Yi Ning Xu

Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China

H

Huai Qin Fu

School of Environment and Science, Gold Coast Campus

X

Xin Yan Li

Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China

J

Jing Jing He

National Enterprise Technology Center Inner Mongolia Erdos Electric Power and Metallurgy Group Company Limited Ordos Inner Mongolia 016064 China

Q

Qiang Niu

J

Jia Chen Wu

Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology 130 Meilong Road Shanghai 200237 China

H

Hai Yang Yuan

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

P

Peng Fei Liu

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

H

Hua Gui Yang

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