膜电极构型CO2还原电解单池的稳定性研究

doi:10.13208/j.electrochem.190305

摘要/Abstract

摘要：

电化学还原CO₂可实现CO₂的资源化转化,是缓解因其过度排放所导致诸多环境问题的关键技术. 本文提出了一种膜电极（membrane electrode assembly,MEA）构型CO₂还原电解单池的结构设计,可同步实现气体扩散阴极两侧CO₂的供给与电解质液层的更新. 基于该MEA构型电解池,实验考察了电解质液层中KHCO₃浓度和更新与否对氮掺杂石墨烯锚定的Ni电极表面CO₂电还原制备CO的反应活性、产物分布与稳定性的影响. 结果表明,若电流密度低于5 mA·cm^-2,KHCO₃浓度显著影响电解电势而非产物分布. CO₂还原电解单池在稳定运行中存在着“可逆”与“不可逆”两种衰减模式. 其中,阴极/电解质界面处催化剂的流失是 “不可逆”衰减形成的原因;而电解质液层中KHCO₃溶液的流失导致了MEA构型CO₂还原单池的“可逆”衰减,周期性更新KHCO₃电解质是降低其“可逆”衰减的有效方法.

关键词: 二氧化碳电还原, 膜电极, 电解池, 稳定性

Abstract:

Electro-catalytic reduction is an efficient way to achieve resourcable transformation of CO₂, which is one of the important techniques to solve the global environmental problems originated from excessive CO₂ emission. In this study, a membrane electrode assembly(MEA) type CO₂ electro-reduction electrolytic cell was constucted, which enables CO₂ feeding and real-time KHCO₃ aqueous updating on both sides of the cathode gas diffusion electrode (GDE). By means of the electrolytic cell, effects of KHCO₃ concentration and updating inside the liquid electrolytic chamber on CO₂ electro-reduction activity, production distribution and stability were investigated. The experimental results suggested that the KHCO₃ concentration exerted strong influence on the cell voltage rather than the production distribution for the current densities lower than 5 mA·cm^-2. The performance of MEA type CO₂ electro-reduction cell decayed in both “reversible” and “irreversible” ways. Catalysts leaking at the GDE/liquid electrolyte interface might be respossible for the cell “irreversible” decay. Meanwhile, th leakage of KHCO₃ aqueous electrolyte arose from gas accumulation in the liquid electrolytic chamber contributed to the “reversible” degradation, which could be recovered effectively by updating the KHCO₃ aqueous electrolyte.

Key words: CO₂ electro-reduction, membrane electrode assembly, electrolytic cell, stability

中图分类号:

O646

毛庆, 李冰玉, 景维云, 赵健, 刘松, 黄延强, 杜兆龙. 膜电极构型CO₂还原电解单池的稳定性研究[J]. 电化学（中英文）, 2020, 26(3): 359-369.

MAO Qing, LI Bing-yu, JING Wei-yun, ZHAO Jian, LIU Song, HUANG Yan-qiang, DU Zhao-long. Stability Studies for a Membrane Electrode Assembly Type CO₂ Electro-Reduction Electrolytic Cell[J]. Journal of Electrochemistry, 2020, 26(3): 359-369.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.190305

https://electrochem.xmu.edu.cn/CN/Y2020/V26/I3/359

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Element/weight%	C	O	F	Al	Si	K	S	Cl	Ni
Start	76.72	1.40	20.84	/	/	/	0.15	0.15	0.74
After 90h	65.35	1.16	33.07	0.07	0.05	0.30	/	/	/

膜电极构型CO₂还原电解单池的稳定性研究

Stability Studies for a Membrane Electrode Assembly Type CO₂ Electro-Reduction Electrolytic Cell

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