多孔炭修饰的吸附催化一体化电极高效电解碳酸氢盐

doi:10.16085/j.issn.1000-6613.2023-1305

化工进展 ›› 2024, Vol. 43 ›› Issue (9): 4892-4899.DOI: 10.16085/j.issn.1000-6613.2023-1305

• 能源加工与技术 • 上一篇

多孔炭修饰的吸附催化一体化电极高效电解碳酸氢盐

王正峰¹(), 谢雨杭²^,³, 李伟科¹, 范永春¹, 康钟尹²^,³, 付乾²^,³()

^1.中国能源建设集团广东省电力设计研究院有限公司，广东广州 510633
^2.重庆大学能源与动力工程学院，重庆 400030
^3.重庆大学工程热物理研究所，重庆 400030

收稿日期:2023-07-30 修回日期:2024-02-18 出版日期:2024-09-15 发布日期:2024-09-30
通讯作者: 付乾
作者简介:王正峰（1983—），男，高级工程师，研究方向为二氧化碳捕集封存及利用、煤炭清洁高效利用。E-mail：wangzhengfeng@gedi.com.cn。
基金资助:
重庆市杰出青年科学基金(cstc2019jcyjjqX0020)

Catalytic adsorption integrated electrode modified by porous carbon for efficient electrolysis of bicarbonate

WANG Zhengfeng¹(), XIE Yuhang²^,³, LI Weike¹, FAN Yongchun¹, KANG Zhongyin²^,³, FU Qian²^,³()

^1.Guangdong Electric Power Design Institute, China Energy Engineering Group, Guangzhou 510633, Guangdong, China
^2.School of Energy and Power Engineering, Chongqing University, Chongqing 400030, China
^3.Institute of Engineering Thermophysics, Chongqing University, Chongqing 400030, China

Received:2023-07-30 Revised:2024-02-18 Online:2024-09-15 Published:2024-09-30
Contact: FU Qian

摘要/Abstract

摘要：

电解碳酸氢盐体系可避免CO₂解吸过程中的能量密集型步骤，更具经济性及技术可行性。但目前阴极存在原位产生CO₂快速逃逸现象，CO₂不能充分参与反应并导致CO₂利用率低等问题，本文将活性炭（activated carbon，AC）作为吸附层修饰电极，与CO₂催化材料Ag均匀混合以构建吸附催化一体化电极，有效调控气体扩散电极孔隙结构，同时探究了不同炭材料的CO₂吸附特性对电解碳酸氢盐性能的影响。在Ag∶AC = 4∶1、Ag纳米颗粒载量为2mg/cm²、全氟磺酸-聚四氟乙烯共聚物（Nafion）质量分数为3.04%时，AC修饰Ag电极具有最高的CO法拉第效率，在100mA/cm²和200mA/cm²电流密度时分别达到59.02%和53.79%。稳定性测试表明该电极能够保持11h的高效运行，CO₂利用率达68.61%。证明了AC修饰的催化吸附一体化电极在电解碳酸氢盐体系中可有效吸附CO₂，提高电化学性能。

关键词: 电化学还原CO₂, 原位还原CO₂, 电解碳酸氢盐, 电极结构, 一体化电极

Abstract:

Electrolytic bicarbonate conversion that can avoid the energy-intensive steps (CO₂ desorption) has attracted particular interest. However, the rapid escape of CO₂ generated in the electrode leads to the insufficient participation of CO₂ in the reaction and the low utilization rate of CO₂. In this study, active carbon (AC) was used as an adsorption layer to modify the electrode. AC was mixed with CO₂ catalytic material Ag to construct an catalytic adsorption integrated electrode (AC+Ag), Which effectively regulated the pore structure of the gas diffusion electrode. And it explored the influence of CO₂ adsorption characteristics of different carbon materials on the performance during the electrolytic bicarbonate conversion. When Ag∶AC was 4∶1, Ag NPs loading was 2mg/cm² and Nafion content was 3.04%, the AC+Ag electrode obtained the highest Faraday efficiency of CO. The FE_CO reached 59.02% and 53.79% at 100mA/cm² and 200mA/cm², respectively. The stability test showed that the electrode can stable convert bicarbonate to CO for 11h. Besides, a high CO₂ utilization rate of 68.61% was obtained. This study proved that the AC-modified catalytic adsorption integrated electrode can effectively adsorb CO₂ in the electrolytic bicarbonate conversion and improve the electrochemical performance.

Key words: electrochemical reduction of CO₂, in situ reduction of CO₂, electrolytic bicarbonate, electrode structure, integrated electrode

中图分类号:

TM911.4

王正峰, 谢雨杭, 李伟科, 范永春, 康钟尹, 付乾. 多孔炭修饰的吸附催化一体化电极高效电解碳酸氢盐[J]. 化工进展, 2024, 43(9): 4892-4899.

WANG Zhengfeng, XIE Yuhang, LI Weike, FAN Yongchun, KANG Zhongyin, FU Qian. Catalytic adsorption integrated electrode modified by porous carbon for efficient electrolysis of bicarbonate[J]. Chemical Industry and Engineering Progress, 2024, 43(9): 4892-4899.

图/表 9

图1 MEA型流动式反应器电解碳酸氢盐系统示意图

图2 电极表面SEM图

图3 Ag、AC、CB的CO2吸附特性和BET测试（1mmHg=133.3224Pa）

图4 不同电极结构电化学性能测试

图5 不同Ag∶AC质量比的样品电化学性能测试

图6 不同浆料配比下样品的电化学性能测试

表1 文献报道的电化学性能参数

CO₂RR 产物	电流密度 /mA·cm^-2	电极名称	反应物	FE_CO/%	参考文献
CO	100	Ag	3mol/L KHCO₃	59.02	本文
CO	100	Ag	3mol/L KHCO₃	48	[9]
CO	100	Ag	3mol/L KHCO₃	37	[14]

图7 电极CO2利用率及稳定性测试

表2 文献报道的CO2利用率

CO₂RR产物	电流密度/mA·cm^-2	CO₂利用率/%	参考文献
CO	50	44.96	本文
CO	50	68.61	本文
CO	100	47.92	本文
CO	200	47.23	本文
CO	180	12.50	[23]
CO	99	4.10	[24]
CO	200	8.20	[24]
CO	190	33.10	[25]
CO	45	7.80	[25]
CO	30	1.00	[25]

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多孔炭修饰的吸附催化一体化电极高效电解碳酸氢盐

Catalytic adsorption integrated electrode modified by porous carbon for efficient electrolysis of bicarbonate

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