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Abstract <p>Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) is a potential technology to facilitate renewable energy storage and reduce carbon emissions. To achieve high selectivity toward value-added carbon commodities at high current density (HCD), unremitting efforts have been made to understand the reaction mechanisms and develop efficient catalysts. However, the computational methods generally lack descriptions of the reaction microenvironment. In this perspective, we discuss the current progress on theoretical analyses for CO<sub>2</sub>RR under HCD and discuss differences between HCD and low current density conditions. The interplay among factors related to catalyst, electrolyte, and electric field is discussed based on a detailed analysis of available experimental data. Finally, an ‘HCD-DFT’ workflow is proposed, which aims to provide a comprehensive theoretical approach to investigate complicated reaction mechanisms, enabling the prediction of selectivity and reconstruction tendency at HCD conditions.</p> Graphical Abstract <p></p> Highlights <p>We point out that the interplay among factors in high current density (HCD) CO2 reduction reaction (CO2RR) systems is more complicated than in low-current-density scenarios. Based on the data analysis, we design a comprehensive workflow incorporating factors associated with catalyst, electrolyte, and electric field for simulating the microenvironment under HCD conditions, which provides a promising approach for mechanistic interpretation and surface reconstruction prediction under HCD.</p> Discussion <p><UnorderedList Mark="Bullet"> <ItemContent> <p>High-value product pathways in CO2RR are promising but often suffer from low selectivity at HCD. The state-of-the-art theoretical analyses lack a proper description of the microenvironment under such conditions. In this work, we fill this gap by conducting a statistical factor analysis comparing HCD and low current density reactions from available experimental data. We propose an 'HCD-DFT' workflow as a comprehensive theoretical methodology for HCD calculations, which includes a potential approach for quantifying current density and surface reconstruction. This workflow not only advances the mechanistic understanding and performance optimization of HCD catalysis in CO2RR but also extends to other electrochemical technologies, thereby accelerating their industrial implementation.</p> </ItemContent> </UnorderedList></p>

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A perspective on mechanism of high-current–density electrocatalytic CO2 reduction

  • 期刊论文

  • 发表日期：

    2025年2月6日

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  • Yumo Chen,
  • Shuqi Hu,
  • Xin Kang,
  • Bilu Liu

摘要

Abstract

Electrochemical CO2 reduction reaction (CO2RR) is a potential technology to facilitate renewable energy storage and reduce carbon emissions. To achieve high selectivity toward value-added carbon commodities at high current density (HCD), unremitting efforts have been made to understand the reaction mechanisms and develop efficient catalysts. However, the computational methods generally lack descriptions of the reaction microenvironment. In this perspective, we discuss the current progress on theoretical analyses for CO2RR under HCD and discuss differences between HCD and low current density conditions. The interplay among factors related to catalyst, electrolyte, and electric field is discussed based on a detailed analysis of available experimental data. Finally, an ‘HCD-DFT’ workflow is proposed, which aims to provide a comprehensive theoretical approach to investigate complicated reaction mechanisms, enabling the prediction of selectivity and reconstruction tendency at HCD conditions.

Graphical Abstract

Highlights

We point out that the interplay among factors in high current density (HCD) CO2 reduction reaction (CO2RR) systems is more complicated than in low-current-density scenarios. Based on the data analysis, we design a comprehensive workflow incorporating factors associated with catalyst, electrolyte, and electric field for simulating the microenvironment under HCD conditions, which provides a promising approach for mechanistic interpretation and surface reconstruction prediction under HCD.

Discussion

High-value product pathways in CO2RR are promising but often suffer from low selectivity at HCD. The state-of-the-art theoretical analyses lack a proper description of the microenvironment under such conditions. In this work, we fill this gap by conducting a statistical factor analysis comparing HCD and low current density reactions from available experimental data. We propose an 'HCD-DFT' workflow as a comprehensive theoretical methodology for HCD calculations, which includes a potential approach for quantifying current density and surface reconstruction. This workflow not only advances the mechanistic understanding and performance optimization of HCD catalysis in CO2RR but also extends to other electrochemical technologies, thereby accelerating their industrial implementation.