一体化电极电催化二氧化碳还原研究进展

引用本文: 宋雨珂, 谢文富, 邵明飞. 一体化电极电催化二氧化碳还原研究进展[J]. 物理化学学报, 2022, 38(6): 210102. doi: 10.3866/PKU.WHXB202101028 shu

Citation: Yuke Song, Wenfu Xie, Mingfei Shao. Recent Advances in Integrated Electrode for Electrocatalytic Carbon Dioxide Reduction[J]. Acta Physico-Chimica Sinica, 2022, 38(6): 210102. doi: 10.3866/PKU.WHXB202101028 shu

一体化电极电催化二氧化碳还原研究进展

北京化工大学化学学院，化工资源有效利用国家重点实验室，北京 100029

作者简介:
谢文富, 2020年毕业于北京化工大学化学专业, 获得博士学位。2020年至今在北京化工大学从事博士后研究。主要研究方向为结构化涉气反应电极设计合成及储能器件;
邵明飞, 2014年于北京化工大学获得博士学位, 期间于2013年获国家公派在牛津大学化学系博士联合培养。现任北京化工大学教授, 博士生导师。主要致力于多维度能源材料设计与合成方法学、新型绿色光电催化化学、结构化电极组装与先进储能器件等研究;

通讯作者: 谢文富, wenfu2010qd@126.com; 邵明飞, shaomf@mail.buct.edu.cn

基金项目:
国家自然科学基金 21922501

国家自然科学基金 22090031

国家自然科学基金 21871021

北京市自然科学基金 2192040

中央高校基本科研业务费专项资金 XK1802-6

中央高校基本科研业务费专项资金 XK1803-05

摘要: 电催化二氧化碳还原反应(E-CO₂RR)可在温和条件下将CO₂转化成高附加值燃料或化学品，近年来受到广泛关注，其在实际反应中涉及到气体扩散和多电子转移等复杂过程，构筑高效、稳定的催化电极是其发展的核心之一。然而，传统涂敷电极制备时，需要将催化剂与粘结剂混合涂覆于集流体表面，此过程会造成活性位点包埋和传质过程受限，致使催化剂活性位利用率下降，同时在反应过程中电极表面容易粉化，造成稳定性下降，难以重复利用。因此，如何调控电极反应界面，提升催化剂活性位的利用率仍面临挑战。将催化剂原位生长于集流体上得到的一体化电极可直接应用于电催化反应，不仅有利于提升活性位利用率以及电荷传输能力，还能有效调控三相界面处的微观反应环境(如pH、反应物及反应中间体的浓度等)，从而实现电催化性能强化。本文综述了一体化电极用于E-CO₂RR的最新进展，分析了结构和表界面调控对E-CO₂RR性能的影响规律，并对该领域仍然存在的挑战和未来一体化E-CO₂RR电极的发展进行了评述与展望。

关键词:

English

Recent Advances in Integrated Electrode for Electrocatalytic Carbon Dioxide Reduction

State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China

Corresponding author: Wenfu Xie, Email: wenfu2010qd@126.com (W.X.); Mingfei Shao, Email: shaomf@mail.buct.edu.cn (M.S.)

Received Date: 15 January 2021
Accepted Date: 22 February 2021
Revised Date: 15 February 2021
Available Online: 15 June 2022
Fund Project:
the National Natural Science Foundation of China

the National Natural Science Foundation of China

the National Natural Science Foundation of China

the Beijing Natural Science Foundation

the Fundamental Research Funds for the Central Universities

the Fundamental Research Funds for the Central Universities

Abstract: The electrocatalytic carbon dioxide reduction reaction (E-CO₂RR) has attracted attention in recent years for its ability to effectively alleviate the environmental problems caused by the rapid increase of CO₂ in the atmosphere and transform CO₂ into high value-added fuels or chemicals (e.g., CO, HCOOH, CH₄, CH₃OH, C₂H₄, C₂H₅OH, etc.) under mild conditions. In addition, clean energy sources, such as solar and wind energy, can provide electrical energy for the electrochemical CO₂ conversion technology used in large-scale industrial applications. One limitation of the E-CO₂RR is that CO₂ is a thermodynamically stable linear molecule with a slow kinetic reaction rate. In addition, the E-CO₂RR involves complex processes, such as gas diffusion and multi-electron transfer, making its selectivity problematic. Therefore, constructing highly efficient and stable catalytic electrodes has become a core research topic in the field of E-CO₂RR. Unfortunately, the traditional method of coating electrodes with binders (e.g., Nafion, polyvinylidene fluoride, and polytetrafluoroethylene) usually results in a low utilization ratio of active sites due to the easy aggregation of the catalysts themselves. This could result in the severe embedding of active sites and limited mass transfer. Moreover, the dissolution of the catalyst layer during the electrocatalytic process also reduces the activity and stability of the electrodes, making it difficult to reuse. Therefore, it is necessary to regulate the electrode reaction interface to improve the utilization ratio of active sites. The integrated electrodes, where the catalyst is grown directly on the current collector, can avoid the use of binders to facilitate the exposure of active sites and transfer of electrons. The integrated structure can also enhance the bonding strength between the active material and current collector and improve the cycling stability of the electrodes. Meanwhile, the micro-environment (e.g., pH, concentration of CO₂, and intermediates) at the three-phase interface can be effectively controlled on the integrated electrodes, which can enhance the performance of the E-CO₂RR. In recent years, encouraging progress has been achieved in the study of the E-CO₂RR. However, current reviews of the E-CO₂RR mainly focus on the regulation of the intrinsic activity of catalysts; discussions and reviews from the perspective of the electrodes are rarely reported. This article reviews the latest research of the integrated electrodes for the E-CO₂RR with a focus on the application of different types of integrated electrodes (e.g., metal, alloy, metal oxide, metal sulfide/phosphide, and metal single atom). It also analyzes the effects of morphology, surface, and interface regulation on the electrocatalytic performance of the E-CO₂RR. Finally, it highlights the challenges that still exist in this field and discusses the future development of the integrated electrodes.

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沈阳化工大学材料科学与工程学院沈阳 110142

一体化电极电催化二氧化碳还原研究进展

通讯作者: 谢文富, wenfu2010qd@126.com; 邵明飞, shaomf@mail.buct.edu.cn

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Recent Advances in Integrated Electrode for Electrocatalytic Carbon Dioxide Reduction

Corresponding author: Wenfu Xie, Email: wenfu2010qd@126.com (W.X.); Mingfei Shao, Email: shaomf@mail.buct.edu.cn (M.S.)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

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CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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中国化学会秘书处

一体化电极电催化二氧化碳还原研究进展

通讯作者: 谢文富, wenfu2010qd@126.com; 邵明飞, shaomf@mail.buct.edu.cn

English

Recent Advances in Integrated Electrode for Electrocatalytic Carbon Dioxide Reduction

Corresponding author: Wenfu Xie, Email: wenfu2010qd@126.com (W.X.); Mingfei Shao, Email: shaomf@mail.buct.edu.cn (M.S.)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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