Structural Design and Performance of Electrocatalysts for Carbon Dioxide Reduction: A Review

doi:10.6023/A21110493

Acta Chimica Sinica ›› 2022, Vol. 80 ›› Issue (2): 199-213.DOI: 10.6023/A21110493 Previous Articles Next Articles

Review

二氧化碳还原电催化剂的结构设计及性能研究进展

李泽洋, 杨宇森^*(), 卫敏

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

投稿日期:2021-11-02 发布日期:2022-01-06
通讯作者: 杨宇森

作者简介:

李泽洋, 北京化工大学在读研究生, 2020年6月于北京化工大学化学学院应用化学专业获得学士学位, 随后加入北京化工大学化工资源有效利用国家重点实验室卫敏教授课题组, 主要研究方向为电催化二氧化碳还原.

杨宇森, 男, 博士, 2014年6月在北京化工大学理学院应用化学专业获得学士学位, 随后加入北京化工大学化工资源有效利用国家重点实验室卫敏教授课题组, 并于2019年6月获得化学工程与技术专业博士学位. 博士阶段主要研究水滑石基负载型催化剂的制备及其对选择性加氢反应的催化性能.

卫敏, 女, 教授, 博士生导师. 2001年于北京大学获理学博士学位. 2008年佐治亚理工学院访问学者. 2001年至今于北京化工大学从事插层化学与功能材料研究. 研究方向: (1)插层结构功能材料的结构设计、组装与性能调控; (2)新型催化材料的结构设计和性能研究. 近5年以通讯作者在J. Am. Chem. Soc.、Angew. Chem., Int. Ed.、Nature Commun.等刊物发表SCI收录研究论文90余篇; 他引11700余次. 2016年入选英国皇家化学会会士; 现担任Science Bulletin期刊副主编, 《催化学报》编委. 获2012年国家杰出青年基金资助. 获2015年中国石油和化学工业联合会科技进步一等奖. 入选2017年度科技部中青年科技创新领军人才和国家百千万人才工程, 被授予“有突出贡献中青年专家”称号. 获2018年第十五届中国青年科技奖.

基金资助:
国家重点研发计划(2021YFC2103501); 国家自然科学基金(22172006); 国家自然科学基金(21521005); 国家自然科学基金(22102006); 北京市自然科学基金(2212012); 中央高校基本科研业务费(XK1802-6); 中央高校基本科研业务费(XK1803-05)

Structural Design and Performance of Electrocatalysts for Carbon Dioxide Reduction: A Review

Zeyang Li, Yusen Yang(), Min Wei

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

Received:2021-11-02 Published:2022-01-06
Contact: Yusen Yang
Supported by:
National Key Research and Development Program of China(2021YFC2103501); National Natural Science Foundation of China(22172006); National Natural Science Foundation of China(21521005); National Natural Science Foundation of China(22102006); Beijing Natural Science Foundation(2212012); Fundamental Research Funds for the Central Universities(XK1802-6); Fundamental Research Funds for the Central Universities(XK1803-05)

With the advance of industrialization of human society, fossil energy has been overconsumed, and excessive carbon dioxide has been discharged into the atmosphere, resulting in energy crisis and environmental issues. The preparation of high value-added fine chemicals by electrocatalytic reduction of carbon dioxide is one of the directions to explore the establishment of artificial carbon cycle, which has attracted extensive attention in fundamental research and industrial applications. Structural design and preparation of electrocatalysts with high activity, selectivity and stability are of great significance to achieve efficient catalytic performance for carbon dioxide reduction. In recent years, many studies have reported the structural design ideas and application cases of catalyst and electrode materials, and remarkable progress has been made. In this review, the regulation strategies of catalyst structure and electrode structure are summarized from four aspects: size effect, surface characteristics, defect engineering and multi-stage structure, and the development of electrocatalytic carbon dioxide reduction is prospected.

Key words: electrocatalytic carbon dioxide reduction, size effect, surface characteristics, defect engineering, multi-stage structure, structural design

Cite this article

Zeyang Li, Yusen Yang, Min Wei. Structural Design and Performance of Electrocatalysts for Carbon Dioxide Reduction: A Review[J]. Acta Chimica Sinica, 2022, 80(2): 199-213.

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Fig. & Tab. 17

Figure 1. Schematic diagram of the goal, approach and strategy of electrocatalytic reduction of carbon dioxide

Half-electrochemical thermodynamic reaction	Electrode potentials (V vs. RHE)
CO₂ (g)+2H⁺+2e→CO(g)+H₂O (1)		–0.106
CO₂ (g)+2H⁺+2e→HCOOH (1)		–0.250
CO₂ (g)+4H⁺+4e→HCHO (1)+H₂O (1)		–0.070
CO₂ (g)+6H⁺+6e→CH₃OH (1)+H₂O (1)		0.016
CO₂ (g)+8H⁺+8e→CH₄ (g)+2H₂O (1)		0.169
2CO₂ (g)+12H⁺+12e→C₂H₄ (g)+4H₂O (1)		0.064
2CO₂ (g)+12H⁺+12→C₂H₅OH (1)+2H₂O (1)		0.084

Table 1. Typical semi-reaction and standard reduction potential of CO2 reduction in aqueous solution (V vs. RHE, pH=7)[21]

Figure 2. TEM images of (a) the 8 nm Au NPs and (b) the C-Au NPs. (c) Potential-dependent FEs of the C-Au on electrocatalytic reduction of CO2 to CO. (d) Current densities for CO formation (mass activities) on the C-Au at various potentials[45]

Figure 3. Density of adsorption sites (yellow, light orange, dark orange, or red symbols for (111), (001), edge, or corner on-top sites, respectively) on closed-shell cuboctahedral Au clusters vs the cluster diameter. The weight fraction of Au bulk atoms is marked with gray dots[45]

Figure 4. TEM and HRTEM images of (a, b) 3.7 nm, (c, d) 6.2 nm and (e, f) 10.3 nm Pd nanoparticles[58]

Figure 5. (a) Ball models of spherical Cu NPs with 2.2 nm and 6.9 nm diameters. Surface atoms are coded according to their first neighbor coordination number (CN), CN<8, CN=8, CN=9, CN>9. (b) Population (relative ratio) of surface atoms with a specific CN as a function of particle diameter[59]

Figure 6. (a) The optimal structure model of Cu(111), Cu13 and Cu13/DG, and the adsorption energy of (b) CO* and (c) H* intermediates[60]

Figure 7. Schematic diagram of synthesis of ultra-thin partial tin oxide alloy catalyst[66]

Figure 8. Sn2.7Cu catalyst (a) SEM diagram; (b) HRTEM diagram; (c) annular dark field-scanning transmission microscope image; and (d) corresponding EDX element distribution map[83]

Figure 9. Schematic diagram of “one bottle, two ships” design and 150 h stability test[6]

Figure 10. Mechanistic investigation of enhanced CH4 production on Ag@Cu2O-6.4NCS (a) Operando ATR-SEIRAS spectra on Ag@Cu2O-6.4 NCs recorded while ramping down the applied potential from –0.6 to –1.3 VRHE. (b, c) Formation energetics of key intermediates *CHO and *COCOH on Cu(111) surface with a *CO coverage of 2/16 ML at 0 V versus RHE (b) and –1.1 V versus RHE (c). (d) Linear scaling relations between *CO coverage and formation energy of *CHO and *COCOH on Cu (111) surface. Insets are the atomistic structure of *CHO under various *CO coverages[10]

Figure 11. Schematic illustration of the electrochemical reconstruction process for ZnO samples[38]

Figure 12. (a) Illustration of the procedures to prepare NPCA. (b) Optical pictures of as-prepared NPCA900. (c) SEM images of NPCA900. (d) TEM and HR-TEM images of NPCA900. (e) Corresponding elemental mappings of NPCA900. (f) XPS spectra of N 1s orbits of NPCA900. (g) XPS spectra of P 2p orbits of NPCA900[81]

Figure 13. The mechanism of the effect of OV on the selectivity of the main product (HCOOH)[94] The mechanism of the effect of OV on the selectivity of the main product (HCOOH)[94]

Figure 14. (a) The XRD spectra of SnO2/CF and OV-SnOx/CF-40 catalysts, (b) Raman spectra, (c) Solid-state EPR spectra, (d, e, f) High-resolution XPS spectra of Sn 3d and O1s, to characterize oxygen vacancies[96] (a) The XRD spectra of SnO2/CF and OV-SnOx/CF-40 catalysts, (b) Raman spectra, (c) Solid-state EPR spectra, (d, e, f) High-resolution XPS spectra of Sn 3d and O1s, to characterize oxygen vacancies[96]

Figure 15. (a) Scheme illustration for the integrated nanostructural NiSn-APC electrode and the CO2RR process on NiSn-APC. SEM images of (b) N-doped carbon nanosheet and (c) NiSn-APC nanoarray[103]

Figure 16. Preparation and structural characterization of electrodes. (A) Process used to prepare various electrodes. (B) SEM image of CP. (C) SEM image of PANI‐CP obtained after electropolymerization for 1 min. (D) SEM image of Cu/PANI‐CP(I) electrodes obtained after metal electrodeposition for 10 min (inset: high‐magnification image). (E) Cross‐section image of the Cu/PANI‐CP(II) electrode. (F) Cross‐section image of the Cu/PANI‐CP(III) electrode (inset: high‐magnification image). (G) SEM image of the Cu‐CP(IV) electrode (inset: high‐magnification image)[102]

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二氧化碳还原电催化剂的结构设计及性能研究进展

Structural Design and Performance of Electrocatalysts for Carbon Dioxide Reduction: A Review

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