铜基催化剂电催化还原CO2制乙醇最新研究进展

doi:10.16085/j.issn.1000-6613.2023-2051

摘要/Abstract

摘要：

CO₂电催化还原技术在能源转换和温室气体减排中具有重要应用潜力。如何获得高电流密度、高选择性的目标产物，尤其是多碳产物，成为该领域的难点和热点。本文综述了铜基催化剂在电催化还原CO₂制乙醇领域的最新研究进展，包括CO₂电催化制乙醇的最高性能水平、催化剂材料的改性策略、电解工艺创新、电极稳定性调控、反应机理等。特别关注了那些能够达到工业应用电流密度且乙醇选择性较高的铜基催化剂的设计、合成和应用。讨论了影响铜基催化剂性能的关键因素，如催化剂的价态、催化剂性能衰减以及电极稳定性等。最后，展望了铜基催化剂在CO₂电催化还原制乙醇领域的未来研究方向，包括提高催化效率、稳定性和工艺放大研究。本文旨在为电催化CO₂还原制乙醇高效催化体系的研发和工业化可行性提供参考和建议。

关键词: 电催化还原, 二氧化碳, 铜, 乙醇, 稳定性, 选择性

Abstract:

The CO₂ electrocatalytic reduction (CO₂ER) technology has a high potential for energy conversion and greenhouse gas reduction. Achieving high current density and desired products with high selectivity, particularly multi-carbon compounds, has become a challenging and hot topic in this field. This article reviews the latest research progress on copper-based catalysts for the electrocatalytic reduction of CO₂ to ethanol, including the excellent performance, catalyst modification strategies, novel electrolysis processes, stability control, and reaction mechanisms. Special emphasis is placed on the design, synthesis, and application of the copper-based catalysts that can achieve industrially relevant current densities and high selectivity for ethanol. The article also discusses the key factors affecting the catalyst performance, such as the catalyst's oxidation state, performance decline, and electrode stability. Finally, it gives prospects for the future research directions of copper-based catalysts for CO₂ER to ethanol, including improving catalytic efficiency, stability and process scale-ups. This article is expected to provide references and suggestions for the development of efficient catalytic systems for CO₂ER to ethanol and their industrialization.

Key words: electrocatalytic reduction, carbon dioxide, copper, ethanol, stability, selectivity

中图分类号:

TQ151.5

佟振伟, 闾菲, 马子然, 李歌, 彭胜攀. 铜基催化剂电催化还原CO₂制乙醇最新研究进展[J]. 化工进展, 2024, 43(12): 6735-6749.

TONG Zhenwei, LYU Fei, MA Ziran, LI Ge, PENG Shengpan. Recent advances in copper-based catalysts for electrocatalytic reduction of CO₂ to ethanol[J]. Chemical Industry and Engineering Progress, 2024, 43(12): 6735-6749.

图/表 12

表1 CO2电催化还原半反应电极电位

反应	电极电位（vs. SHE）/V
2H⁺+2e^- $\overset{}{\to}$ H₂	-0.42
CO₂+8H^-+8e^- $\overset{}{\to}$ CH₄+2H₂O	-0.24
CO₂+6H⁺+6e^- $\overset{}{\to}$ CH₃OH+H₂O	-0.38
CO₂+4H⁺+4e^- $\overset{}{\to}$ HCHO+H₂O	-0.51
CO₂+2H⁺+2e^- $\overset{}{\to}$ CO+H₂O	-0.52
CO₂+2H⁺+2e^- $\overset{}{\to}$ HCOOH	-0.61
2CO₂+12H⁺+12e^- $\overset{}{\to}$ C₂H₄+4H₂O	0.064
2CO₂+12H⁺+12e^- $\overset{}{\to}$ C₂H₅OH+3H₂O	0.084

表1 CO2电催化还原半反应电极电位

反应	电极电位（vs. SHE）/V
2H⁺+2e^- $\overset{}{\to}$ H₂	-0.42
CO₂+8H^-+8e^- $\overset{}{\to}$ CH₄+2H₂O	-0.24
CO₂+6H⁺+6e^- $\overset{}{\to}$ CH₃OH+H₂O	-0.38
CO₂+4H⁺+4e^- $\overset{}{\to}$ HCHO+H₂O	-0.51
CO₂+2H⁺+2e^- $\overset{}{\to}$ CO+H₂O	-0.52
CO₂+2H⁺+2e^- $\overset{}{\to}$ HCOOH	-0.61
2CO₂+12H⁺+12e^- $\overset{}{\to}$ C₂H₄+4H₂O	0.064
2CO₂+12H⁺+12e^- $\overset{}{\to}$ C₂H₅OH+3H₂O	0.084

图1 铜基催化剂电催化还原CO2生成多碳产物的机理[粗实线为H2（ΔG*H=0，12H2⇌ *H）和CO（ΔG*CO=0，CO⇌ *CO）的热力学吸脱附平衡条件]

图2 CuAu、Cu/Au和Cu上CO2还原的路径和机理[28]

图3 P-Cu x /Cu2OF催化电极上三种不同表面位点的反应机理示意图（左）以及在-0.7V vs. RHE时，Cu(‍Ⅰ‍)/Cu(0)摩尔比和位点对不同主产物选择性影响（右）[32]

图4 Cu CF催化剂的性能[16]

图5 V掺杂的Cu2Se纳米管生长过程的示意图及Cu1.22V0.19Se的SEM、TEM图和XPS谱图[37]

图6 金属掺杂铜基催化剂的CO2电还原制乙醇的性能和中间产物

图7 铜基分子催化剂的性能和结构[44]

图8 氮掺杂碳层改性的Cu催化剂的CO2还原性能[45]

表2 近期铜基催化剂CO2ER制备乙醇产物的最新活性数据总结

催化剂	电流密度/A·cm^-2	FE_乙醇/%	电位/V vs. RHE	膜种类	电解液	电解池类型	稳定时间/h	参考文献
LA Cu₂O	0.4	25	—	—	2mol/L KCl	流动池	2	[15]
Cu ^δ⁺	0.4	48.1	-2.88	阴膜	0.02mol/L KHCO₃	MEA	10	[16]
CuAu	0.3	60	-0.75	—	0.1mol/L KHCO₃	流动池	90	[28]
V-Cu₂Se	0.2	68	-0.8	—	0.1mol/L KHCO₃	流动池	140	[37]
BaO/Cu	0.4	45	-0.75	阴膜	1mol/L KOH	流动池	20	[39]
F-Cu	1.6	15	-0.9	阴膜	1mol/L KOH	流动池	40	[42]
FeTPP[Cl]/Cu	0.124	41	-0.82	—	1mol/L KHCO₃	流动池	2	[44]
N-C/Cu	0.156	52	-0.68	阴膜	1mol/L KOH	流动池	—	[45]
Ce(OH) _x -Cu	0.128	43	-0.7	阴膜	1mol/L KOH	流动池	6	[49]
CuO _x @C	0.164	45	-1	—	1mol/L KOH	流动池	50	[51]
Ag/Cu₂O	0.32	40	-0.87	阴膜	1mol/L KOH	流动池	6	[52]

图9 两步法CO2电化学还原过程示意图[53]

图10 聚合物基气体扩散电极的结构和性能[61]

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铜基催化剂电催化还原CO₂制乙醇最新研究进展

Recent advances in copper-based catalysts for electrocatalytic reduction of CO₂ to ethanol

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