电催化二氧化碳还原制备气态产物的研究进展

doi:10.11949/0438-1157.20240094

摘要/Abstract

摘要：

随着工业化进程的快速推进，CO₂排放量预计将持续上升，CO₂捕获、储存和再利用受到研究者们的广泛关注。在各类CO₂转化技术中，电催化技术因其反应条件温和可控、能耗低、环境污染小等优点，是最有前途的策略之一。近些年来，CO₂选择性地转化为气态产物如一氧化碳、合成气、甲烷、乙烯和乙烷已有许多报道。本文对电催化CO₂还原生成气体产物的反应机理和催化剂设计策略进行了介绍；对电催化CO₂还原进行了总结与展望，包括新型电催化剂、机理研究、外部因素的影响以及级联反应。

关键词: 电催化CO₂还原, 气态产物, 反应机理, 催化剂设计策略

Abstract:

With the rapid advancement of industrialization, CO₂ emissions are expected to continue to rise, and carbon dioxide capture, storage and reuse have been received widespread attention from researchers. In various CO₂ conversion technologies, electrocatalytic technology is one of the most promising strategies because of its mild and controllable reaction conditions, low energy consumption and low environmental pollution. In recent years, there have been many reports on the selective conversion of CO₂ into gaseous products such as carbon monoxide, syngas, methane, ethylene and ethane. In this paper, the reaction mechanism and catalyst design strategies of electrocatalytic CO₂ reduction to gas products are introduced. The electrocatalytic CO₂ reduction is summarized and prospected, including new electrocatalysts, mechanism studies, the influence of external factors and cascade reactions.

Key words: electrocatalytic CO₂ reduction, gas products, reaction mechanism, catalyst design strategies

中图分类号:

TQ 151.5⁺2

刘旭升, 李泽洋, 杨宇森, 卫敏. 电催化二氧化碳还原制备气态产物的研究进展[J]. 化工学报, 2024, 75(7): 2385-2408.

Xusheng LIU, Zeyang LI, Yusen YANG, Min WEI. Research progress on electrocatalytic carbon dioxide reduction to gaseous products[J]. CIESC Journal, 2024, 75(7): 2385-2408.

图/表 13

图1 电化学能量转换及研究示意图

Fig.1 Schematic diagram of electrochemical energy conversion and research

表1 水溶液中CO2还原反应可能发生的代表性半反应和标准还原电位［20］

Table 1 Typical semi-reaction and standard reduction potential that may occur for CO2 reduction in aqueous solution［20］

反应	反应方程式	标准氢电极电势(vs SHE)/V
ECO₂RR半反应	CO₂(g) + 2H⁺+ 2e^- $\overset{}{\to}$ CO(g) +H₂O (1)	-0.106
	CO₂(g) + 2H⁺+ 2e^- $\overset{}{\to}$ HCOOH (1)	-0.250
	CO₂(g) + 4H⁺+ 4e^- $\overset{}{\to}$ HCHO (1) + H₂O (1)	-0.070
	CO₂(g) + 6H⁺+ 6e^- $\overset{}{\to}$ CH₃OH (1) + H₂O (1)	0.016
	CO₂(g) + 8H⁺+ 8e^- $\overset{}{\to}$ CH₄ (g) + 2H₂O (1)	0.169
	2CO₂(g) + 12H⁺+ 12e^- $\overset{}{\to}$ C₂H₄ (g) + 4H₂O (1)	0.064
	2CO₂(g) + 12H⁺+ 12e^- $\overset{}{\to}$ C₂H₅OH (1) + 3H₂O (1)	0.084
	2CO₂(g) + 2H⁺+ 2e^- $\overset{}{\to}$ H₂C₂O₄(aq)	-0.05
HER半反应	2H₂O(g) + 2e^-→ H₂ (g) + 2OH^- (aq)	0

表1 水溶液中CO2还原反应可能发生的代表性半反应和标准还原电位［20］

Table 1 Typical semi-reaction and standard reduction potential that may occur for CO2 reduction in aqueous solution［20］

反应	反应方程式	标准氢电极电势(vs SHE)/V
ECO₂RR半反应	CO₂(g) + 2H⁺+ 2e^- $\overset{}{\to}$ CO(g) +H₂O (1)	-0.106
	CO₂(g) + 2H⁺+ 2e^- $\overset{}{\to}$ HCOOH (1)	-0.250
	CO₂(g) + 4H⁺+ 4e^- $\overset{}{\to}$ HCHO (1) + H₂O (1)	-0.070
	CO₂(g) + 6H⁺+ 6e^- $\overset{}{\to}$ CH₃OH (1) + H₂O (1)	0.016
	CO₂(g) + 8H⁺+ 8e^- $\overset{}{\to}$ CH₄ (g) + 2H₂O (1)	0.169
	2CO₂(g) + 12H⁺+ 12e^- $\overset{}{\to}$ C₂H₄ (g) + 4H₂O (1)	0.064
	2CO₂(g) + 12H⁺+ 12e^- $\overset{}{\to}$ C₂H₅OH (1) + 3H₂O (1)	0.084
	2CO₂(g) + 2H⁺+ 2e^- $\overset{}{\to}$ H₂C₂O₄(aq)	-0.05
HER半反应	2H₂O(g) + 2e^-→ H₂ (g) + 2OH^- (aq)	0

图2 (a)ECO2RR形成CO示意图；(b) Cr2O9H4/Ag(111)和Ag(111)生成CO的自由能图[42]

Fig.2 (a) Schematic diagram of ECO2RR formation of CO; (b) Free energy diagram of Cr2O9H4/Ag(111) and Ag(111) to generate CO[42]

图3 (a) np-Au的多孔网络结构以及形成的pH梯度[50]；(b) Au NW和Au NP的边缘位置质量分数作为Au原子数的函数以及边缘/角的理想化比率[51]；(c) 中空多孔Ag球形催化剂的合成示意图及SEM图像[53]；(d) Tri-Ag NPs合成示意图[54]；(e) Pd八面体和Pd二十面体的HAADF-STEM图像[56]；(f) CO2在Pd(111)、Pd(211)、Pd55和Pd38上还原为CO的自由能图[57]

Fig.3 (a) The porous network structure of np-Au and the pH gradient formed[50]; (b) The percentage of mass at the edge position of Au NW and Au NP as a function of the number of Au atoms and the idealization ratio of the edge/angle[51]; (c) Schematic diagram and SEM images of the synthesis of hollow porous Ag spherical catalyst[53]; (d) Schematic diagram of Tri-Ag NPs synthesis[54]; (e) HAADF-STEM images of Pd octahedron and Pd icosahedral[56]; (f)Free energy diagram of CO2 reduced to CO on Pd(111), Pd(211), Pd55 and Pd38[57]

图4 (a) 多孔网络结构的SEM图及性能[59]；(b) Zn枝晶的原位XANES数据[60]；(c) Cu-Sn纳米颗粒合成及结构表征[64]；(d) Cu-In的SEM及EDS图像[65]；(e) NCNT的物理特性[68]；(f) 煤转化为N掺杂多孔碳催化剂的示意图及性能对比[69]；(g) 缺陷石墨烯（DG）的合成及其对CO2的电催化还原的示意图[70]

Fig.4 (a) SEM image and performance of porous network structure[59]; (b) In-situ XANES data of Zn dendrite[60]; (c) Synthesis and structural characterization of Cu-Sn nanoparticles[64]; (d) SEM and EDS images of Cu-In[65]; (e) Physical properties of NCNT[68]; (f) Schematic diagram and performance comparison of coal to N doped porous carbon catalysts[69]; (g) Synthesis of defective graphene (DG) and its electrocatalytic reduction of CO2[70]

图5 (a) AuCu合金催化剂还原CO2示意及性能[72]；(b) Au/TiNS不同电压下H2与CO比例的范围[74]；(c) Ag/TiO2催化剂不同电位下H2/CO比例[77]；(d) ZIF-8负载Ag纳米颗粒BET等温线和FTIR图像 [80]；(e) Pd-SnO2形成示意图[81]；(f) PdMo-CNSs催化性能[82]

Fig.5 (a) Schematic diagram and performance of AuCu alloy catalyst for CO2 reduction[72]; (b) Range of H2 to CO ratio at different voltages of Au/TiNS[74]; (c) H2/CO ratio of Ag/TiO2 catalyst at different potentials[77]; (d) ZIF-8 loaded Ag nanoparticle BET isotherm and FTIR image[80]; (e) Schematic diagram of Pd-SnO2 formation[81]; (f) Catalytic performance of PdMo-CNSs[82]

图6 (a) R-Cu3P/Cu、O-Cu3P/Cu和Cu3P/Cu的高分辨率XPS谱图[84]；(b) 碳掺杂缺陷ZnO火焰合成装置示意[85]；(c) PNC的SEM、HRTEM图像和EDS谱图[87]；(d) pCNTA的催化性能[88]

Fig.6 (a) High-resolution XPS spectra of R-Cu3P/Cu, O-Cu3P/Cu and Cu3P/Cu[84]; (b) Schematic diagram of ZnO flame synthesis device with carbon doping defect[85]; (c) SEM, HRTEM images and EDS spectra of PNC[87]; (d) Catalytic performance of pCNTA[88]

图7 (a)ECO2RR形成CH4示意图；(b) Cu(211)表面CO2转化为CH4自由能图[94]

Fig.7 (a) Schematic diagram of ECO2RR formation of CH4; (b) Free energy diagram of CO2 conversion to CH4 over Cu(211) surfaces[94]

图8 (a) Cu/Al2O3 SAC和Cu/Cr2O3 SAC上的ECO2RR的自由能图[100]；(b) Cu SAs/GDY形成的示意图及形貌表征[101]；(c) BNC-Cu的SEM、TEM图像以及EDS谱图[102]；(d) 不同尺寸的八面体Cu纳米晶体TEM图像以及相应尺寸统计分析[104]；(e) 疏水碳涂层铜核壳结构及其催化机理示意图[105]；(f) tw-Cu催化剂的结构表征[106]

Fig.8 (a) Free energy plots of ECO2RR on Cu/Al2O3 SAC and Cu/Cr2O3 SAC[100]; (b) Schematic diagram and morphological characterization of Cu SAs/GDY formation[101]; (c) SEM, TEM images and EDS spectra of BNC-Cu[102]; (d) TEM images of octahedral Cu nanocrystals of different sizes and statistical analysis of corresponding sizes[104]; (e) Schematic diagram of hydrophobic carbon-coated copper core-shell structure and its catalytic mechanism[105]; (f) Structural characterization of tw-Cu catalysts[106]

图9 (a) CuAg NWs的制备示意图[108]；(b) CuPd催化剂在不同比例下的形态演变[109]；(c) 一锅法合成SnCu x O2+x @MFI的示意图[110]；(d) Cu-CeO x 和CuO/CeO2在不同电势下的原位ATR-IR光谱[111]

Fig.9 (a) Schematic of preparing CuAg NWs[108]; (b) Schematic diagram and morphological characterization of Cu SAs/GDY formation[109]; (c) Schematic diagram of the synthesis of SnCu x O2+x @MFI by one-pot method[110]; (d) In situ ATR-IR spectra on Cu-CeO x and CuO/CeO2 at different potentials[111]

图10 (a) ECO2RR形成C2H4示意图；(b) Cu(111)表面CO2转化为C2H4自由能图[123]

Fig.10 (a) Schematic diagram of ECO2RR formation of C2H4; (b) Free energy diagram of CO2 conversion to C2H4 over Cu(111) surfaces[123]

图11 (a) 用FS-ALD生成Al2O3包覆的Cu纳米晶体的示意及性能[128]；(b) C2H4在Cu2O不同晶面上形成及性能[129]；(c)立方Cu2O和支链CuO的性能 [130]；(d) 具有不同曲率的铜基催化剂的制备过程示意图 [131]；(e) Cu 纳米立方体和纳米球体的TEM图像及XRD谱图[132]；(f) 44 nm Cu NC立方体的平面位点和边缘位点之间存在最佳平衡[132]

Fig.11 (a) Schematic diagram and performance of Al2O3 coated Cu nanocrystals generated by FS-ALD[128]; (b) Formation and properties of C2H4 on different crystal planes of Cu2O[129]; (c) Performance of cubic Cu2O and branched CuO [130]; (d) Schematic diagram of the preparation process of copper-based catalysts with different curvatures [131]; (e) TEM images and XRD patterns of Cu nanocubes and nanospheres[132]; (f) An optimal balance between planar and edge sites of the 44 nm Cu NC cube[132]

图12 (a) Cu纳米线的TEM图像[133]；(b) Al-Cu2O 的XPS谱图[134]；(c) CuLaCs三金属电催化剂性能[135]；(d) CuAg双金属催化剂的形态及物相表征[137]；(e) Cu/ZnO串联催化剂的性能[138]；(f) Zn@Cu-NWAs 的合成示意图 [144]；(g) xFe2O3-N@CN的合成示意图[124]

Fig.12 (a) TEM image of Cu nanowires[133]; (b) XPS spectra of Al-Cu2O[134]; (c) Properties of CuLaCs trimetallic electrocatalysts[135]; (d) Morphological characterization of CuAg bimetallic catalyst[137]; (e) Performance of Cu/ZnO tandem catalysts[138]; (f) Synthesis diagram of Zn@Cu-NWAs[144]; (g) Synthesis diagram of xFe2O3-N@CN[124]

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