电解工艺条件对Cu基催化剂电化学还原CO2的产物分布影响

doi:10.11896/cldb.23100052

材料导报

2024, Vol. 38

Issue (24): 23100052-5 https://doi.org/10.11896/cldb.23100052

无机非金属及其复合材料

电解工艺条件对Cu基催化剂电化学还原CO₂的产物分布影响

高娜¹, 庞佩琦², 李智³, 牟国栋³, 崔天成¹, 杜贤龙¹, 李涛², 肖国萍^1,*

1 中国科学院上海应用物理研究所,中国科学院微观界面物理与探测重点实验室,上海 201800
2 华东理工大学大型工业反应器工程教育部工程中心,上海 200237
3 山东能源集团有限公司大型煤气化及煤基新材料国家工程中心,济南 250000

Study of Process Parameters Effects on Product Distribution of CO₂ Electroreduction over Cu-based Catalysts

GAO Na¹, PANG Peiqi², LI Zhi³, MOU Guodong³, CUI Tiancheng¹, DU Xianlong¹, LI Tao², XIAO Guoping^1,*

1 Key Laboratory of Interfacial Physics and Technology, Chinese Academy of Sciences, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China
2 Engineering Research Center of Large Scale Reactor Engineering and Technology, Ministry of Education, East China University of Science and Technology, Shanghai 200237, China
3 National Engineering Research Center of Coal Gasification and Coal-Based Advanced Materials, Shan Dong Energy Group Co., Ltd.,Jinan 250000, China

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摘要工业化发展实现生产力飞跃的同时,化石能源的消耗导致大气中二氧化碳(CO₂)含量升高,电化学还原CO₂(CO₂RR)制备高附加值化学品,不仅能解决温室气体带来的问题,还能够缓解能源危机。铜基催化剂是目前用于CO₂RR的有效催化剂之一,本研究通过对铜片表面水热处理制备氧化亚铜,将CO₂电化学还原为甲酸和一氧化碳,并系统性考察了电解液浓度、CO₂压力以及电解液温度对电化学还原产物分布的影响。实验结果发现,电解液浓度降低、CO₂压力增加可以抑制析氢反应,电解液温度升高有利于CO的生成。当电解液浓度1 mol/L、温度30 ℃,CO₂的压力为55 atm时,在-0.7～-1.2 V (vs.RHE)测试电压范围内,甲酸法拉第效率达70%以上,最高达可到83.6%。当电解液温度由30 ℃升至80 ℃,电压为-0.9 V(vs.RHE)时,甲酸法拉第效率由80%降低到49.7%,CO法拉第效率由4.4%增加到39.2%,表明随着电解液温度升高,甲酸法拉第效率降低。

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	高娜
	庞佩琦
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	牟国栋
	崔天成
	杜贤龙
	李涛
	肖国萍

关键词: 电化学还原二氧化碳铜基催化剂甲酸一氧化碳

Abstract: With industrial thriving development, the consumption of fossil energy has increased the carbon dioxide (CO₂) content in the atmosphere, and the preparation of high value-added chemicals by electroreduction of CO₂ (CO₂RR) not only solves the problems caused by greenhouse gases, but also can alleviate the energy crisis. Copper-based catalyst is one of the effective catalysts currently used for CO₂RR. In this work, Cu₂O was prepared by hydrothermal treatment of copper sheet surface to CO₂RR to formic acid and carbon monoxide, and the effects of electrolyte concentration, CO₂ pressure, and electrolyte temperature on the distribution of electrochemical reduction products were systematically investigated. It was found that the decrease of electrolyte concentration and the increase of CO₂ pressure could inhibit the hydrogen evolution reaction, and the increase of electrolyte temperature was favorable for the generation of CO. When the electrolyte concentration was 1 mol/L, the temperature was 30 ℃, and the pressure of CO₂ was 55 atm, the formic acid Faraday efficiency reached more than 70% and up to 83.6% in the -0.7—-1.2 V (vs. RHE) test voltage range. When the electrolyte temperature increased from 30 ℃ to 80 ℃ at -0.9 V (vs.RHE), the formic acid Faraday efficiency decreases from 80% to 49.7%, while the CO Faraday efficiency increases from 4.4% to 39.2%, which shows that the formic acid Faraday efficiency decreases with the increase of electrolyte temperature.

Key words: electrochemical reduction carbon dioxide copper catalyst HCOOH CO

出版日期: 2024-12-25 发布日期: 2024-12-20

ZTFLH:

TQ150

基金资助: 山东省重点研发计划(2020CXGC010402);中国科学院上海应用物理研究所育新计划项目(SINAP-YXJH-2022008)

通讯作者: * 肖国萍,中国科学院上海应用物理研究所正研级高级工程师、博士研究生导师。2006年哈尔滨工程大学化学工程与工艺专业本科毕业,2012年华东理工大学化学工程专业博士毕业后到中国科学院上海应用物理研究所工作至今。目前主要从事二氧化碳电化学还原以及电解水制氢的研究工作。发表论文30余篇,包括IECR、Fuel和Science China Chemistry等。 xiaoguoping@sinap.ac.cn

作者简介: 高娜,2012年中国石油大学(华东)化学工程与工艺专业本科毕业,2016年石油化工科学研究院工业催化专业硕士研究生毕业。2019年1月入职中国科学院上海应用物理研究所至今,主要从事二氧化碳电化学还原制备高附加值化学品的研究工作。

引用本文:

高娜, 庞佩琦, 李智, 牟国栋, 崔天成, 杜贤龙, 李涛, 肖国萍. 电解工艺条件对Cu基催化剂电化学还原CO₂的产物分布影响[J]. 材料导报, 2024, 38(24): 23100052-5.
GAO Na, PANG Peiqi, LI Zhi, MOU Guodong, CUI Tiancheng, DU Xianlong, LI Tao, XIAO Guoping. Study of Process Parameters Effects on Product Distribution of CO₂ Electroreduction over Cu-based Catalysts. Materials Reports, 2024, 38(24): 23100052-5.

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http://www.mater-rep.com/CN/10.11896/cldb.23100052 或 http://www.mater-rep.com/CN/Y2024/V38/I24/23100052

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