脉冲策略强化SnO_(x)电极长效还原CO_(2)制甲酸机理研究  

Mechanism of Long-term Reduction of CO_(2)to Formic Acid on SnO_(x)Electrode Enhanced by Pulse Strategy

作　　者：蒋浩 朱德圣[2] 闫喜凤 于洋茜 郑飞 赵黎明 杨金明 刘妍 罗仙平[1,2] JIANG Hao;ZHU Desheng;YAN Xifeng;YU Yangxi;ZHENG Fei;ZHAO Liming;YANG Jinming;LIU Yan;LUO Xianping(State Key Laboratory of Nuclear Resources and Environment,East China University of Technology,Nanchang 330013,China;School of Water Resources and Environmental Engineering,East China University of Technology,Nanchang 330013,China)

机构地区：[1]东华理工大学核资源与环境国家重点实验室,江西南昌330013 [2]东华理工大学水资源与环境工程学院,江西南昌330013

出　　处：《东华理工大学学报(自然科学版)》2024年第6期601-608,共8页Journal of East China University of Technology(Natural Science)

基　　金：赣鄱俊才支持计划-主要学科学术和技术带头人培养项目(20232BCJ23097);江西省自然科学基金项目(20224BAB-203028)。

摘　　要：SnO_(x)是电催化还原二氧化碳制甲酸的高效活性催化剂,然而,在传统恒电位还原CO_(2)过程中会被还原成低价金属氧化物或零价金属,导致活性降低甚至失活。脉冲电催化技术可以动态调控电极表面活性物质,且操作简单,可利用脉冲策略来强化SnO_(x)催化剂的稳定性。实验结果表明,脉冲电位条件下,SnO_(x)电极在电解12 h后仍保持良好的稳定性,制甲酸法拉第效率维持在40%左右,比恒电位条件下高153%。结合物化表征与电化学测试结果可知,SnO_(x)催化稳定性归因于脉冲氧化电位促使电极表面SnO_(x)原位动态再生,并促进活性组分分散。研究成果为提高金属氧化物电极电催化还原CO_(2)制甲酸的稳定性提供了一种新的技术思路。SnO_(x)is an efficient and active catalyst for the electrochemical reduction of carbon dioxide to produce formate.However,under traditional constant-potential CO_(2)reduction,SnO_(x)tends to be reduced to lower-valent metal oxides or elemental metals,leading to decreased activity or even deactivation.The pulsed electrocatalysis technique enables dynamic regulation of active species on the electrode surface and it is easy to operate.Therefore,a pulsed strategy to enhance the catalyst stability of SnO_(x)is used in the study.Experimental results indicate that under pulsed potential conditions,the SnO_(x)electrode maintains good stability after 12 hours of electrolysis,with a Faradaic efficiency for formate production of approximately 40%,an improvement of 153%compared to constant-potential conditions.Based on physicochemical characterization and electrochemical testing,the outstanding catalytic stability is attributed to the pulsed oxidation potential,which promotes dynamic in-situ regeneration of SnO_(x)on the electrode surface and facilitates the dispersion of active components.The research results provide a novel technical approach to enhance the stability of metal oxide electrodes for electrocatalytic CO_(2)reduction to formate.

关 键 词：二氧化碳 还原 锡氧化物 脉冲电催化 

分 类 号：O646.5[理学—物理化学]