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

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

Abstract

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

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

CLC Number:

TM911.4

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.

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.

Figures/Tables 9

References 25

1	SANCHEZ Felipe, MOTTA Davide, ROLDAN Alberto, et al. Hydrogen generation from additive-free formic acid decomposition under mild conditions by Pd/C: Experimental and DFT studies[J]. Topics in Catalysis, 2018, 61(3): 254-266.
2	AGARWAL Arun S, ZHAI Yumei, HILL Davion, et al. The electrochemical reduction of carbon dioxide to formate/formic acid: Engineering and economic feasibility[J]. ChemSusChem, 2011, 4(9): 1301-1310.
3	BUSHUYEV Oleksandr S, DE LUNA Phil, DINH Cao Thang, et al. What should we make with CO₂ and how can we make it?[J]. Joule, 2018, 2(5): 825-832.
4	Rern Jern LIM, XIE Mingshi, Mahasin Alam SK, et al. A review on the electrochemical reduction of CO₂ in fuel cells, metal electrodes and molecular catalysts[J]. Catalysis Today, 2014, 233: 169-180.
5	LARRAZÁBAL Gastón O, Patrick STRØM-HANSEN, HELI Jens P, et al. Analysis of mass flows and membrane cross-over in CO₂ reduction at high current densities in an MEA-type electrolyzer[J]. ACS Applied Materials & Interfaces, 2019, 11(44): 41281-41288.
6	BOOT-HANDFORD Matthew E, ABANADES Juan C, ANTHONY Edward J, et al. Carbon capture and storage update[J]. Energy & Environmental Science, 2014, 7(1): 130-189.
7	WANG Yuan, ZHAO Li, OTTO Alexander, et al. A review of post-combustion CO₂ capture technologies from coal-fired power plants[J]. Energy Procedia, 2017, 114: 650-665.
8	Stuart HASZELDINE R. Carbon capture and storage: How green can black be?[J]. Science, 2009, 325(5948): 1647-1652.
9	LI Tengfei, LEES Eric W, GOLDMAN Maxwell, et al. Electrolytic conversion of bicarbonate into CO in a flow cell[J]. Joule, 2019, 3(6): 1487-1497.
10	YUE Pengtao, KANG Zhongyin, FU Qian, et al. Life cycle and economic analysis of chemicals production via electrolytic (bi)carbonate and gaseous CO₂ conversion[J]. Applied Energy, 2021, 304: 117768.
11	REYES Angelica, JANSONIUS Ryan P, MOWBRAY Benjamin A W, et al. Managing hydration at the cathode enables efficient CO₂ electrolysis at commercially relevant current densities[J]. ACS Energy Letters, 2020, 5(5): 1612-1618.
12	WHEELER Danika G, MOWBRAY Benjamin A W, REYES Angelica, et al. Quantification of water transport in a CO₂ electrolyzer[J]. Energy & Environmental Science, 2020, 13(12): 5126-5134.
13	LI Yuguang C, ZHOU Dekai, YAN Zhifei, et al. Electrolysis of CO₂ to syngas in bipolar membrane-based electrochemical cells[J]. ACS Energy Letters, 2016, 1(6): 1149-1153.
14	LEES Eric W, GOLDMAN Maxwell, FINK Arthur G, et al. Electrodes designed for converting bicarbonate into CO[J]. ACS Energy Letters, 2020, 5(7): 2165-2173.
15	SHODIEV Abbos, ZANOTTO Franco M, YU Jia, et al. Designing electrode architectures to facilitate electrolyte infiltration for lithium-ion batteries[J]. Energy Storage Materials, 2022, 49: 268-277.
16	SING K S W. Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity [J]. Pure and Applied Chemistry, 1985, 57(4): 603-619.
17	KIBRIA Md Golam, EDWARDS Jonathan P, GABARDO Christine M, et al. Electrochemical CO₂ reduction into chemical feedstocks: From mechanistic electrocatalysis models to system design[J]. Advanced Materials, 2019, 31(31): 1807166.
18	MAREPALLY Bhanu Chandra, AMPELLI Claudio, GENOVESE Chiara, et al. Enhanced formation of >C₁ products in electroreduction of CO₂ by adding a CO₂ adsorption component to a gas-diffusion layer-type catalytic electrode[J]. ChemSusChem, 2017, 10(22): 4442-4446.
19	WENG Lien-Chun, BELL Alexis T, WEBER Adam Z. Modeling gas-diffusion electrodes for CO₂ reduction[J]. Physical Chemistry Chemical Physics, 2018, 20(25): 16973-16984.
20	HIGGINS Drew, HAHN Christopher, XIANG Chengxiang, et al. Gas-diffusion electrodes for carbon dioxide reduction: A new paradigm[J]. ACS Energy Letters, 2019, 4(1): 317-324.
21	HYUN Gayea, SONG Jun Tae, Changui AHN, et al. Hierarchically porous Au nanostructures with interconnected channels for efficient mass transport in electrocatalytic CO₂ reduction[J]. Proceedings of the National Academy of Sciences of the United States of America, 2020, 117(11): 5680-5685.
22	WU Jingjie, SHARMA Pranav P, HARRIS Bradley H, et al. Electrochemical reduction of carbon dioxide: Ⅳ dependence of the Faradaic efficiency and current density on the microstructure and thickness of tin electrode[J]. Journal of Power Sources, 2014, 258: 189-194.
23	HAAS Thomas, KRAUSE Ralf, WEBER Rainer, et al. Technical photosynthesis involving CO₂ electrolysis and fermentation[J]. Nature Catalysis, 2018, 1: 32-39.
24	VERMA Sumit, HAMASAKI Yuki, KIM Chaerin, et al. Insights into the low overpotential electroreduction of CO₂ to CO on a supported gold catalyst in an alkaline flow electrolyzer[J]. ACS Energy Letters, 2018, 3(1): 193-198.
25	KUTZ Robert B, CHEN Qingmei, YANG Hongzhou, et al. Sustainion imidazolium-functionalized polymers for carbon dioxide electrolysis[J]. Energy Technology, 2017, 5(6): 929-936.

[1]	FENG Zhanxiong, ZHANG Chuang, LIU Dezheng, WANG Yun, MA Qiang, WANG Cheng. Effect of different atmosphere heat treatment on the oxygen reduction performance of Pt/C catalysts prepared by continuous pipeline microwave technology [J]. Chemical Industry and Engineering Progress, 2024, 43(6): 3080-3092.
[2]	LAN Ruisong, LIU Lihua, ZHANG Qian, CHEN Boyan, HONG Junming. Performance and biotoxicity evaluation of sulfur-doped graphene as a cathode for MFC [J]. Chemical Industry and Engineering Progress, 2024, 43(6): 3430-3439.
[3]	ZHANG Bao, WANG Peng, AN Yongpan, LYU Ping, JIANG Jianliang. Design and experiment of fuel cell systems for marine application [J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2554-2567.
[4]	FANG Yao, LIU Lei, GAO Zhihua, HUANG Wei, ZUO Zhijun. Advances in anode catalysts for photo-assisted direct methanol fuel cells [J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2611-2628.
[5]	ZHU Taizhong, ZHANG Liang, HUANG Zequan, LUO Lingping, HUANG Fei, XUE Lixin. Preparation and characterization of gel polybenzimidazole proton exchange membrane with alkyl sulfonic acid side chains [J]. Chemical Industry and Engineering Progress, 2024, 43(4): 1962-1971.
[6]	FENG Zhanxiong, WANG Yun, MA Qiang, ZHANG Chuang, WANG Cheng. Preparation of Pt/C catalyst by continuous pipeline microwave technology and its oxygen reduction performance [J]. Chemical Industry and Engineering Progress, 2022, 41(12): 6377-6384.
[7]	PAN Wenzheng, JI Zhiyong, WANG Jing, LI Shuming, HUANG Zhihui, GUO Xiaofu, LIU Jie, ZHAO Yingying, YUAN Junsheng. Research on the electricity production performance and degradation process of microbial fuel cell treating azo-dye saline wastewater [J]. Chemical Industry and Engineering Progress, 2022, 41(6): 3306-3313.
[8]	LI Dan, ZHANG Boya, LIU Bohong, TAO Yang, XIONG Zi’ang, HOU Sanying. Research progress on low platinum load and high stable membrane electrode assembly of proton exchange membrane fuel cell [J]. Chemical Industry and Engineering Progress, 2021, 40(S2): 89-100.
[9]	LI Yunfei, WANG Zhipeng, DUAN Lei, CHEN Liang, XU Shoudong, ZHANG Ding, DUAN Donghong, LIU Shibin. Research progress of ordered membrane electrode assembly for proton exchange membrane fuel cells [J]. Chemical Industry and Engineering Progress, 2021, 40(S1): 101-110.
[10]	LIAO Peiyi, YANG Daijun, MING Pingwen, XUE Mingzhe, LI Bing, ZHANG Cunman. Research progress of gas-liquid two-phase flow in micro-channel and its application in PEMFC [J]. Chemical Industry and Engineering Progress, 2021, 40(9): 4734-4748.
[11]	HE Guangli, DOU Meiling. Progress on effect of hydrogen impurities on the performance of automotive fuel cells [J]. Chemical Industry and Engineering Progress, 2021, 40(9): 4815-4822.
[12]	MA Zifeng, HE Yijun, CHEN Jianfeng. Renewable energy chemical engineering and technology [J]. Chemical Industry and Engineering Progress, 2021, 40(9): 4687-4695.
[13]	LIU Pengcheng, XU Sichuan. Experimental study on dynamic response performance for PEMFC stack [J]. Chemical Industry and Engineering Progress, 2021, 40(6): 3172-3180.
[14]	Xiaomin LIU, Bangqiang ZHANG, Bin AI, Yanmei YANG, Juan WANG, Haibo YANG, Hong CAI, Wei BAO. Development and current status of hydrogen quality standards for proton exchange membrane fuel cell [J]. Chemical Industry and Engineering Progress, 2021, 40(2): 703-708.
[15]	Zexue DU. Application advances of manufacturing technology for key materials of vehicle fuel cell stack [J]. Chemical Industry and Engineering Progress, 2021, 40(1): 6-20.