CO2电催化还原产合成气研究进展

doi:10.16085/j.issn.1000-6613.2021-2009

摘要/Abstract

摘要：

CO₂电催化还原产合成气是通过CO₂资源化利用实现碳中和的有效途径之一，但仍存在过电位高、选择性差、难以精准调控合成气组成比例等问题。本文综述了CO₂电催化还原产合成气的催化剂研究进展，包括金属催化剂、金属配合物催化剂、金属氧化物及硫化物催化剂、金属单原子催化剂以及非金属催化剂等；进一步地，概述了H型电解池、连续流电解池、固体氧化物电解池以及膜反应器电解池等电化学反应池特征。在此基础上，总结了提升CO₂电催化还原产合成气效率的有效策略，包括阳极反应耦合、双活性位催化剂结构设计以及催化剂多级形貌调控等。最后探讨了CO₂电催化还原产合成气领域未来的发展方向：通过机器学习辅助催化剂设计筛选；结合多尺度模拟理解电化学界面过程；利用原位表征技术探究反应机理等。

关键词: 二氧化碳, 电催化, 还原, 合成气, 催化剂

Abstract:

Electrocatalytic CO₂ reduction to syngas is one of the effective ways to realize CO₂ utilization, but some problems, such as high overpotential, poor selectivity and difficulty in accurately regulating the composition of syngas, still exist in its application. This paper reviews the research progresses of the electrocatalysts for CO₂ reduction to syngas, including metal catalysts, metal complex catalysts, metal oxide and sulfide catalysts, as well as single atom catalysts and non-metallic catalysts. Furthermore, the characteristics of H-type cell, continuous flow cell, solid oxide electrolytic cell and membrane reactor electrolytic cell are introduced. Also, effective strategies to improve the catalytic efficiency of CO₂ electroreduction to syngas are summarized, including anodic reaction coupling, structure design of double-active site catalysts and control of catalysts' hierarchical morphology. Finally, the future development directions of syngas production by CO₂ electroreduction are discussed, including machine learning aided catalyst design, understanding the interfacial electrochemical process with multi-scale simulation and exploring the reaction mechanism using operando characterizations.

Key words: carbon dioxide, electrocatalysis, reduction, syngas, catalysts

中图分类号:

O643.36

华亚妮, 冯少广, 党欣悦, 郝文斌, 张保文, 高展. CO₂电催化还原产合成气研究进展[J]. 化工进展, 2022, 41(3): 1224-1240.

HUA Yani, FENG Shaoguang, DANG Xinyue, HAO Wenbin, ZHANG Baowen, GAO Zhan. Research progress of CO₂ electrocatalytic reduction to syngas[J]. Chemical Industry and Engineering Progress, 2022, 41(3): 1224-1240.

图/表 13

表1 电化学还原CO2半反应的电极电位（标准试验条件）[10]

电化学半反应	电极电位（vs. SHE）/V
$2 H + + 2 e → H 2$	-0.42
$C O 2 + 2 H + + 2 e - → C O + H 2 O$	-0.52
$C O 2 + 2 H + + 2 e - → H C O O H$	-0.61
$C O 2 + 4 H + + 4 e - → H C H O + H 2 O$	-0.51
$C O 2 + 6 H + + 6 e - → C H 3 O H + H 2 O$	-0.38
$C O 2 + 8 H + + 8 e - → C H 4 + 2 H 2 O$	-0.24
$2 C O 2 + 12 H + + 12 e - → C 2 H 4 + 4 H 2 O$	0.064
$2 C O 2 + 12 H + + 12 e - → C 2 H 5 O H + 3 H 2 O$	0.084

表1 电化学还原CO2半反应的电极电位（标准试验条件）[10]

电化学半反应	电极电位（vs. SHE）/V
$2 H + + 2 e → H 2$	-0.42
$C O 2 + 2 H + + 2 e - → C O + H 2 O$	-0.52
$C O 2 + 2 H + + 2 e - → H C O O H$	-0.61
$C O 2 + 4 H + + 4 e - → H C H O + H 2 O$	-0.51
$C O 2 + 6 H + + 6 e - → C H 3 O H + H 2 O$	-0.38
$C O 2 + 8 H + + 8 e - → C H 4 + 2 H 2 O$	-0.24
$2 C O 2 + 12 H + + 12 e - → C 2 H 4 + 4 H 2 O$	0.064
$2 C O 2 + 12 H + + 12 e - → C 2 H 5 O H + 3 H 2 O$	0.084

图1 电极表面电催化反应过程

图2 金纳米颗粒催化活性

图3 银纳米颗粒制备过程及催化机理[30]

图4 锌纳米颗粒电催化还原二氧化碳

图5 镍配合物电催化还原二氧化碳[46]

图6 钌配合物催化剂电化学还原CO2产合成气[47]

图7 典型的H型CO2电还原系统

图8 合金催化剂电还原CO2

图9 高温CO2电解的碳循环过程[79]

图10 基于双极膜电解池的CO2电还原技术[89]

图11 阳极反应耦合阴极CO2还原反应

图12 碳多级结构

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CO₂电催化还原产合成气研究进展

Research progress of CO₂ electrocatalytic reduction to syngas

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