The Role of Phase Mixing Degree in Promoting C−C Coupling in Electrochemical CO2 Reduction Reaction on Cu-based Catalysts

Yinuo Wang; Fei Yang; Hongming Xu; Juhee Jang; Ernest P. Delmo; Xiaoyi Qiu; Zhehan Ying; Ping Gao; Shangqian Zhu; M. Danny Gu; Minhua Shao

doi:10.1002/anie.202400952

The Role of Phase Mixing Degree in Promoting C−C Coupling in Electrochemical CO₂ Reduction Reaction on Cu-based Catalysts

Yinuo Wang
, Fei Yang
, Hongming Xu
, Juhee Jang
, Ernest P. Delmo
, Xiaoyi Qiu
, Zhehan Ying
, Ping Gao
, Shangqian Zhu^*
, M. Danny Gu^*
, Minhua Shao^*

^*Corresponding author for this work

Department of Chemistry

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

39 Citations (Scopus)

29 Downloads (CityUHK Scholars)

Abstract

Cu-based catalysts have been identified as the most promising candidates for generation of C2+ products in electrochemical CO₂ reduction reaction. Defect engineering in catalysts is a widely employed strategy for promoting C−C coupling on Cu. However, comprehensive understanding of defect structure-to-activity relationship has not been obtained. In this study, controllable defects generation is achieved, which leads to a series of Cu-based catalysts with various phase mixing degrees. It is observed that the Faradaic efficiency toward C2+ products increases with the phase mixing degree, reaching 81 % at maximum. In situ infrared absorption spectroscopy reveals that the catalysts with higher phase mixing degree tend to form *CO more easily and possess higher retention of *CO under high overpotential window, thereby promoting C−C coupling. This work sheds new light on the relationship between defects and C−C coupling, and the rational developed of more advanced Cu-base catalysts.

© 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

Original language	English
Article number	e202400952
Number of pages	8
Journal	Angewandte Chemie - International Edition
Volume	63
Issue number	16
Online published	19 Feb 2024
DOIs	https://doi.org/10.1002/anie.202400952
Publication status	Published - 15 Apr 2024

Funding

edgements This work was supported by the Research Grants Council (16304821, 16310419 and 16308420), Innovation and Technology Commission (grant no. ITC-CNERC14EG03) of the Hong Kong Special Administrative Region. S. Zhu was supported by the Start-up Research Fund of Southeast University (RF1028623256). This work was also supported by the Material Characterization and Preparation Facility (GZ) of Hong Kong University of Science and Technology (Guangzhou).The authors acknowledge N. Ho from HKUST for XPS me

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 13 Climate Action

Research Keywords

C2+ generation
CO2 reduction reaction
defects management
infrared spectrum

Publisher's Copyright Statement

This full text is made available under CC-BY-NC 4.0. https://creativecommons.org/licenses/by-nc/4.0/

RGC Funding Information

RGC-funded

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Cite this

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title = "The Role of Phase Mixing Degree in Promoting C−C Coupling in Electrochemical CO2 Reduction Reaction on Cu-based Catalysts",

abstract = "Cu-based catalysts have been identified as the most promising candidates for generation of C2+ products in electrochemical CO2 reduction reaction. Defect engineering in catalysts is a widely employed strategy for promoting C−C coupling on Cu. However, comprehensive understanding of defect structure-to-activity relationship has not been obtained. In this study, controllable defects generation is achieved, which leads to a series of Cu-based catalysts with various phase mixing degrees. It is observed that the Faradaic efficiency toward C2+ products increases with the phase mixing degree, reaching 81 \% at maximum. In situ infrared absorption spectroscopy reveals that the catalysts with higher phase mixing degree tend to form *CO more easily and possess higher retention of *CO under high overpotential window, thereby promoting C−C coupling. This work sheds new light on the relationship between defects and C−C coupling, and the rational developed of more advanced Cu-base catalysts. {\textcopyright} 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",

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AU - Yang, Fei

AU - Xu, Hongming

AU - Jang, Juhee

AU - Delmo, Ernest P.

AU - Qiu, Xiaoyi

AU - Ying, Zhehan

AU - Gao, Ping

AU - Zhu, Shangqian

AU - Gu, M. Danny

AU - Shao, Minhua

PY - 2024/4/15

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N2 - Cu-based catalysts have been identified as the most promising candidates for generation of C2+ products in electrochemical CO2 reduction reaction. Defect engineering in catalysts is a widely employed strategy for promoting C−C coupling on Cu. However, comprehensive understanding of defect structure-to-activity relationship has not been obtained. In this study, controllable defects generation is achieved, which leads to a series of Cu-based catalysts with various phase mixing degrees. It is observed that the Faradaic efficiency toward C2+ products increases with the phase mixing degree, reaching 81 % at maximum. In situ infrared absorption spectroscopy reveals that the catalysts with higher phase mixing degree tend to form *CO more easily and possess higher retention of *CO under high overpotential window, thereby promoting C−C coupling. This work sheds new light on the relationship between defects and C−C coupling, and the rational developed of more advanced Cu-base catalysts. © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

AB - Cu-based catalysts have been identified as the most promising candidates for generation of C2+ products in electrochemical CO2 reduction reaction. Defect engineering in catalysts is a widely employed strategy for promoting C−C coupling on Cu. However, comprehensive understanding of defect structure-to-activity relationship has not been obtained. In this study, controllable defects generation is achieved, which leads to a series of Cu-based catalysts with various phase mixing degrees. It is observed that the Faradaic efficiency toward C2+ products increases with the phase mixing degree, reaching 81 % at maximum. In situ infrared absorption spectroscopy reveals that the catalysts with higher phase mixing degree tend to form *CO more easily and possess higher retention of *CO under high overpotential window, thereby promoting C−C coupling. This work sheds new light on the relationship between defects and C−C coupling, and the rational developed of more advanced Cu-base catalysts. © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

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KW - defects management

KW - infrared spectrum

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