物理化学学报 >> 2022, Vol. 38 >> Issue (11): 2206020.doi: 10.3866/PKU.WHXB202206020

所属专题: 新锐科学家专刊

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铜基串联催化剂电催化CO2还原的研究进展

石永霞, 侯曼, 李俊俊, 李丽, 张志成()   

  • 收稿日期:2022-06-14 录用日期:2022-07-12 发布日期:2022-07-20
  • 通讯作者: 张志成 E-mail:zczhang19@tju.edu.cn
  • 基金资助:
    国家自然科学基金(22071172)

Cu-Based Tandem Catalysts for Electrochemical CO2 Reduction

Yongxia Shi, Man Hou, Junjun Li, Li Li, Zhicheng Zhang()   

  • Received:2022-06-14 Accepted:2022-07-12 Published:2022-07-20
  • Contact: Zhicheng Zhang E-mail:zczhang19@tju.edu.cn
  • About author:Zhicheng Zhang, Email: zczhang19@tju.edu.cn; Tel.: +86-15822798044
  • Supported by:
    the National Natural Science Foundation of China(22071172)

摘要:

化石燃料的燃烧和其他人类活动排放了大量的CO2气体,引发了诸多环境问题。电催化CO2还原反应(CO2RR)可以储存间歇可再生能源,实现人为闭合碳循环,被认为是获得高附加值化学品和燃料的有效途径。电催化CO2RR涉及多个电子-质子转移步骤,其中*CO通常被认为是关键中间体。铜由于对*CO具有合适的吸附能,已被广泛证明是唯一能够有效地将CO2还原为碳氢化合物和含氧化合物的金属催化剂。然而,纯Cu稳定性差、产品选择性低、过电位高,阻碍了工业级多碳产品的生产。构筑Cu基串联催化剂是提高CO2RR性能的一种有前途的策略。本文首先介绍电催化CO2RR的反应路线和串联机理。然后,系统地总结铜基串联催化剂对电催化CO2RR的最新研究进展。最后,提出合理设计和可控合成新型电催化CO2RR串联催化剂面临的挑战和机遇。

关键词: CO2还原, 铜, 串联催化剂, 溢流, 电催化

Abstract:

Through the combustion of fossil fuels and other human activities, large amounts of CO2 gas have been emitted into the atmosphere, causing many environmental problems, such as the greenhouse effect and global warming. Thus, developing and utilizing renewable clean energy is crucial to reduce CO2 emission and achieve carbon neutrality. The electrochemical CO2 reduction reaction (CO2RR) has been considered as an effective approach to obtain high value-added chemicals and fuels, which can store intermittent renewable energy and achieve the artificial carbon cycle. In addition, due to its multiple advantages, such as mild reaction conditions, tunable products, and simple implementation, electrochemical CO2RR has attracted extensive attention. Electrochemical CO2RR involves multiple electron–proton transfer steps to obtain multitudinous products, such as C1 products (CO, HCOOH, CH4, etc.) and C2 products (C2H4, C2H5OH, etc.). The intermediates, among which *CO is usually identified as the key intermediate, and reaction pathways of different products intersect, resulting in an extremely complex reaction mechanism. Currently, copper has been widely proven to be the only metal catalyst that can efficiently reduce CO2 to hydrocarbons and oxygenates due to its suitable adsorption energy for *CO. However, the low product selectivity, poor stability, and high overpotential of pure Cu hinder its use for the production of industrial-grade multi-carbon products. Tandem catalysts with multiple types of active sites can sequentially reduce CO2 molecules into desired products. When loaded onto a co-catalyst that can efficiently convert CO2 to *CO (such as Au and Ag), Cu acts as an electron donor owing to its high electrochemical potential. *CO species generated from the substrate can spillover onto the surface of electron-poor Cu due to the stronger adsorption and be further reduced to C2+ products. The use of Cu-based tandem catalysts for electrochemical CO2RR is a promising strategy for improving the performance of CO2RR and thus, has become a research hotspot in recent years. In this review, we first introduce the reaction routes and tandem mechanisms of electrochemical CO2RR. Then, we systematically summarize the recent research progress of Cu-based tandem catalysts for electrochemical CO2RR, including Cu-based metallic materials (alloys, heterojunction, and core-shell structures) as well as Cu-based framework materials, carbon materials, and polymer-modified materials. Importantly, the preparation methods of various Cu-based tandem catalysts and their structure–activity relationship in CO2RR are discussed and analyzed in detail. Finally, the challenges and opportunities of the rational design and controllable synthesis of advanced tandem catalysts for electrochemical CO2RR are proposed.

Key words: CO2 reduction, Cu, Tandem catalyst, Spillover, Electrocatalysis

MSC2000: 

  • O646