CO2电化学还原制CO金属催化剂的研究进展

doi:10.3969/j.issn.1006-396X.2022.06.006

摘要/Abstract

摘要：

利用可再生能源CO₂电化学还原制CO是实现“碳中和”目标及可再生能源储存的有效途径之一。简述了CO₂电化学还原的优势及基本反应原理，综述了近年来水溶液中CO₂电化学还原制CO金属电催化剂的研究进展。从制备纳米粒子并调控其组成和结构、构筑合金、设计金属中心和配体与载体的结构以及开发单原子催化剂等方面，重点讨论了单金属纳米催化剂、双金属催化剂、金属有机络合物催化剂和单原子催化剂对CO₂电化学还原制CO性能的影响及相关反应机理，总结了各类催化剂的优缺点，对CO₂电化学还原制CO金属催化剂的发展方向进行了展望。

关键词: 二氧化碳, 电化学还原, 一氧化碳, 电催化剂

Abstract:

Electrochemical reduction of CO₂ to CO using renewable energy is one of the effective ways to achieve "carbon neutrality" and renewable energy storage.This review briefly described the advantages and basic principles of the electrochemical reduction of CO₂ and summarized the research progress of metal electrocatalysts for the electrochemical reduction of CO₂ to CO in aqueous solutions in recent years.Specifically,this study mainly introduced the recent research progress of mono?metal nanocatalysts,bimetallic catalysts,metal?organic complex catalysts,and mono?atom catalysts,which included their influences on the electrochemical reduction of CO₂ and relevant reaction mechanisms.The introduction was conducted from several perspectives,such as the preparation of nanoparticles as well as the regulation of their composition and structure,alloy construction,structural design of metal centers as well as their ligands and carriers,and the development of mono?atom catalysts. In addition, this study summarized the advantages and disadvantages of various catalysts and predicted the development trend of metal catalysts.

Key words: Carbon dioxide, Electrochemical reduction, Carbon monoxide, Electrocatalyst

中图分类号:

TQ15

范琳, 杨磊, 车晓甄, 李夺, 潘立卫, 钟和香. CO₂电化学还原制CO金属催化剂的研究进展[J]. 石油化工高等学校学报, 2022, 35(6): 48-58.

Lin Fan, Lei Yang, Xiaozhen Che, Duo Li, Liwei Pan, Hexiang Zhong. Research Progress of Metal Catalysts for Electrochemical Reduction of CO₂ to CO[J]. Journal of Petrochemical Universities, 2022, 35(6): 48-58.

图/表 8

表1 ERC阴极反应及对应的标准电极电位

Table 1 ERC cathode reaction and corresponding standard electrode potential

反应方程式	电极电位（vs.NHE）/V
CO₂+e^-→CO $2 • -$	-1.90
CO₂+2H⁺+2e^-→CO+H₂O	-0.53
CO₂+2H⁺+2e^-→HCOOH	-0.61
CO₂+4H⁺+4e^-→HCHO+H₂O	-0.48
CO₂+6H⁺+6e^-→CH₃OH+H₂O	-0.38
CO₂+8H⁺+8e^-→CH₄+H₂O	-0.24
2H⁺+2e^-→H₂	-0.41

表1 ERC阴极反应及对应的标准电极电位

Table 1 ERC cathode reaction and corresponding standard electrode potential

反应方程式	电极电位（vs.NHE）/V
CO₂+e^-→CO $2 • -$	-1.90
CO₂+2H⁺+2e^-→CO+H₂O	-0.53
CO₂+2H⁺+2e^-→HCOOH	-0.61
CO₂+4H⁺+4e^-→HCHO+H₂O	-0.48
CO₂+6H⁺+6e^-→CH₃OH+H₂O	-0.38
CO₂+8H⁺+8e^-→CH₄+H₂O	-0.24
2H⁺+2e^-→H₂	-0.41

图1 CO2电催化还原制CO示意图

Fig.1 Schematic diagram of electrocatalytic reduction of CO2 to CO

表2 单金属纳米催化剂ERC制CO性能对比

Table 2 Comparison of ERC to CO performance of single metal nanocatalysts

催化剂	电解液	电位（vs.RHE)/V	j_CO/(mA·cm^-2)	FE_CO/%	文献
Pd NPs	0.1 mol/L KHCO₃	-0.89	16.00	91.2	[18]
Au NPs	0.1 mol/L KHCO₃	-1.20	-	45.0	[19]
Au TOH	0.1 mol/L KHCO₃	-0.60	-	88.8	[20]
L25‐Ag‐NCs	0.1 mol/L KHCO₃	-0.86	5.90	99.0	[21]
Pd concave cubes	0.1 mol/L KHCO₃	-0.90	-	90.0	[22]
D‐25Ag NWs	0.1 mol/L KHCO₃	-0.96	6.65	699.3	[23]
SPC‐Ag	0.1 mol/L KHCO₃	-0.90	23.80	93.0	[24]
ED Zn	0.5 mol/L KHCO₃	-1.10	16.00	77.9	[25]
w‐Zn	0.5 mol/L KHCO₃	-0.95	40.00	98.0	[26]

表3 双金属催化剂ERC制CO性能对比

Table 3 Comparison of ERC to CO performance of bimetallic catalysts

催化剂	电解液	电位（vs.RHE）/V	j_CO/(mA·cm^-2)	FE_CO/%	稳定性/h	文献
Cu₂Cd/Cd/Cu	0.1 mol/L KHCO₃	-1.00	8.00	84.0	126	[30]
CuIn₂₀	0.1 mol/L KHCO₃	-0.60	-	93.0	0	[31]
Pd_0.8Au	0.5 mol/L KHCO₃	-0.60	-	94.3	8	[32]
AuFe‐CSNPs	0.5 mol/L KHCO₃	-0.40	19.70	97.6	901	[33]
3D‐h Cu‐Sn	0.1 mol/L KHCO₃	-0.45	9.60	98.6	0	[34]
In‐doped Cu@Cu₂O	0.1 mol/L KHCO₃	-0.80	11.10	87.6	4	[35]
Zn‐Cu	0.1 mol/L KHCO₃	-0.96	3.40	97.0	20	[36]
Ag₇₀Pd₃₀	0.1 mol/L KHCO₃	-0.80	9.30	98.6	8	[37]

图2 AuFe?CSNPs结构演化示意图及其结构表征

Fig.2 Structural evolution diagram and characterizations of AuFe?CSNPs

表4 金属有机络合物催化剂ERC制CO性能对比

Table 4 Comparison of ERC to CO performance of metal?organic complex catalysts

催化剂	电解液	电位(vs.RHE)/V	j_CO/（mA·cm^-2）	FE_CO/%	稳定性/h	文献
CoPc/CNT	0.1 mol/L KHCO₃	-0.60	12.00	>90.0	15	[41]
CoPc⁃py⁃CNT	0.2 mol/L NaHCO₃	-0.63	9.90	>98.0	12	[42]
FePGF	0.1 mol/L KCl	-0.59	-	93.0	24	[43]
NiPc⁃OMe⁃MDE	0.5 mol/L KHCO₃	-0.50	150.00	>99.5	40	[44]
CoPc2	0.5 mol/L NaHCO₃	-0.65	70.50	94.0	10	[45]
CoPc(CN)₈	0.1 mol/L KHCO₃	-0.52	15.00	>95.0	10	[46]
NiPc⁃TFPN⁃COF	0.5 mol/L KHCO₃	-0.90	16.30	99.8	60	[47]

表5 单原子催化剂ERC制CO性能对比

Table 5 Comparison of ERC to CO performance of monoatomic catalysts

催化剂	电解液	电位（vs.RHE）/V	j_CO/(mA·cm^-2)	FE_CO/%	稳定性/h	文献
Ni SACs	0.5 mol/L KHCO₃	-0.80	10.00	97.0	-	[50]
Fe³⁺‐N‐C/GDE	0.5 mol/L KHCO₃	-0.45	94.00	>90.0	12	[51]
Fe_0.5d	0.1 mol/L KHCO₃	-0.60	7.50	91.0	-	[52]
C‐Zn1Ni₄ZIF‐8	1.0 mol/L KHCO₃	-0.63	71.50±2.90	97.8	12	[53]
Ni₅‐PTF‐1000	0.5 mol/L KHCO₃	-0.90	18.40	94.0	16	[54]
Fe/NG‐750	0.1 mol/L KHCO₃	-0.57	-	~80.0	10	[55]
Co‐N₂ SACs	0.5 mol/L KHCO₃	-0.68	18.10	95.0	60	[56]
NiSA‐N₂‐C	0.5 mol/L KHCO₃	-0.80	-	98.0	10	[57]

图3 Ni x ‐PTF‐1000单原子催化剂合成示意图

Fig.3 Schematic views of the fabrication of Ni x ?PTF?1000 catalyst

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CO₂电化学还原制CO金属催化剂的研究进展

Research Progress of Metal Catalysts for Electrochemical Reduction of CO₂ to CO

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