二氧化碳还原电催化剂的结构设计及性能研究进展

doi:10.6023/A21110493

化学学报 ›› 2022, Vol. 80 ›› Issue (2): 199-213.DOI: 10.6023/A21110493 上一篇下一篇

综述

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)

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摘要/Abstract

随着人类社会工业化进程的推进, 化石能源被过度消耗, 人类向大气中排放过量的二氧化碳, 造成能源危机和环境问题. 通过电催化二氧化碳还原反应来制备高附加值精细化学品是积极探索建立人工碳循环的方向之一, 引起了基础研究与工业应用领域研究者的广泛关注. 设计与制备具有高活性、高选择性和高稳定性的电催化剂对于实现二氧化碳高效还原具有重要意义. 近年来, 关于催化剂与电极材料的结构设计和应用案例有许多报道, 取得了显著的进步. 分别从尺寸效应、表面特性、缺陷工程和多级结构四个方面对催化剂结构与电极结构的调控策略进行了综述, 并对电催化二氧化碳还原领域的发展进行了展望.

关键词: 电催化二氧化碳还原, 尺寸效应, 表面特性, 缺陷工程, 多级结构, 结构设计

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

引用此文

李泽洋, 杨宇森, 卫敏. 二氧化碳还原电催化剂的结构设计及性能研究进展[J]. 化学学报, 2022, 80(2): 199-213.

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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图/表 17

图1. 电催化二氧化碳还原目标、途径和策略的示意图

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

表1. 水溶液中CO2还原反应的代表性半反应和标准还原电位(相对可逆氢电极, pH=7)[21]

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

图2. (a) 8 nm Au纳米颗粒和(b) C-Au纳米颗粒的TEM图像. (c) C-Au对CO2电催化还原为CO的电位依赖性. (d)不同电位下C-Au上CO生成(质量活度)的电流密度[45]

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]

图3. 立方八面体Au团簇上吸附位置(黄色、浅橙色、深橙色或红色符号, 分别代表(111)、(001)、边或角的顶部位置)的密度与团簇直径的关系. 金体相原子的重量分数用灰色圆点标记[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]

图4. (a, b) 3.7 nm, (c, d) 6.2 nm和(e, f) 10.3 nm Pd颗粒的TEM图像和HRTEM图像[58]

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]

图5. (a)球形Cu纳米粒子的球形模型, 直径分别为2.2和6.9 nm. 表面原子根据其第一邻位配位数(CN)进行编码, CN<8, CN=8, CN=9, CN>9. (b)具有特定CN的表面原子概率(相对比率)与颗粒直径的函数[59]

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]

图6. (a) Cu(111)、Cu13和Cu13/DG (defective graphene)优化结构模型, (b) CO*和(c) H*中间体的吸附能[60]

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]

图7. 超薄部分氧化锡合金催化剂的合成示意图[66]

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

图8. Sn2.7Cu催化剂的(a) SEM图; (b) HRTEM图; (c)环形暗场-扫描透射显微镜图像, 以及(d)相应EDX元素分布图[83]

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]

图9. “一瓶两船”设计示意图及150 h稳定性测试[6]

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

图10. Ag@Cu2O-6.4NCS上甲烷生成增强的机理研究(a)在催化剂Ag@Cu2O-6.4NCS上记录的ATR-SEIRAS谱在外加电位从–0.6 VRHE降至–1.3 VRHE. (b, c)关键中间体*CHO和*COCOH在Cu(111)表面的生成能, 在0 VRHE (b)和–1.1 VRHE (c), 其中*CO覆盖度均为2/16 ML. (d) *CO覆盖度与*CHO和*COCOH在Cu(111)表面的生成能之间存在线性标度关系. 插入图是*CHO在各种*CO覆盖度下的原子结构[10]

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]

图11. 氧化锌样品的电化学重建过程示意图[38]

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

图12. (a)制备NPCA的流程图. (b)制备的NPCA900的光学照片. (c) NPCA900的扫描电镜图像. (d) NPCA900的TEM和HR-TEM图像. (e) NPCA900的相应元素映射. (f) NPCA900的N 1s轨道的XPS谱. (g) NPCA900的P 2p轨道的XPS谱[81]

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]

图13. OV对主产物(HCOOH)选择性影响的机理[94]

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]

图14. SnO2/CF和OV-SnOx/CF-40催化剂的(a)XRD图谱, (b)拉曼光谱, (c)固体EPR谱, (d) Sn 3d和(e, f) O 1s的高分辨XPS谱, 用于表征氧空位[96]

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]

图15. (a)一体化电极结构NiSn-APC的制备工艺和用于CO2RR示意图, (b) N掺杂碳纳米片和(c) NiSn-APC纳米阵列的SEM图[103]

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]

图16. (A)用于制备各种电极的工艺. (B) CP的扫描电镜图像. (C)电聚合1 min后得到的PANI-CP的扫描电镜图像. (D) Cu/PANI-CP(I)电极在金属电沉积10 mim后的扫描电镜图像(插图: 高倍率图像). (E) Cu/PANI-CP(II)电极的截面图像. (F) Cu/PANI-CP(III)电极的截面图像(插图: 高倍率图像). (G) Cu-Cp(IV)电极的扫描电镜图像(插图: 高倍率图像)[102]

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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