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化学工业与工程 2016, Vol. 33 Issue (5) :8-13    DOI: 10.13353/j.issn.1004.9533.20141019
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多孔锡电极的制备及其用于CO2电化学还原性能
韩真真, 王华, 王静, 韩金玉
天津大学化工学院, 绿色合成与转化教育部重点实验室, 天津 300072
Fabrication of Porous Tin and Its Application to Electroreduction of CO2
Han Zhenzhen, Wang Hua, Wang Jing, Han Jinyu
Key laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

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摘要 

用氢气泡动态模板法在铜基底上沉积锡制备了一种新型锡电极。采用SEM、EDS和XRD对多孔锡沉积层进行表征,并对其催化CO2电化学还原制甲酸的性能进行了研究。SEM结果表明多孔锡沉积层具有自组织的蜂窝状三维多孔结构,同时EDS分析表明电极表面无杂质。XRD表征表明在基底和Sn沉积层交界处有Cu5Sn6合金生成,加强了两者之间的连接。采用不同扫描速率下循环伏安曲线法测试电化学表面积,多孔锡电极的电化学表面积大约是普通锡片电极的6倍。电极的循环伏安测试结果表明,多孔锡电极比普通锡片电极具有更高的电流密度,更正的起峰电位,说明具有多孔结构的电极对CO2电化学还原反应具有更高的活性。通过考察KHCO3浓度、还原电位对还原过程的影响,确定KHCO3浓度为0.5 mol/L,还原电位为-1.7 V vs.SCE时,甲酸的电流效率可达73.9%。由此可见,多孔结构电极材料能有效地提高CO2电还原的催化效果。

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韩真真
王华
王静
韩金玉
关键词多孔锡电极;   二氧化碳;   电化学还原;   电流密度;   电流效率     
Abstract

The porous tin electrode was fabricated by hydrogen bubbles evolution using Cu as substrate. It was characterized by SEM, EDS and XRD, and its application to electroreduction of CO2 to formic acid was investigated. SEM revealed that a kind of self-assembly distribution constructed honeycomb-like porous network, and EDS indicated that there were no impurities. XRD revealed that there was Sn-Cu intermetallic compound layer at the interface between tin deposit layer and copper, which can enhance the bonding force of the two. Cyclic voltammetry curves at different scan rates indicated that its electroactive surface area was six times higher than that of the commercial Sn electrode. Cyclic voltammetry curves of two electrodes demonstrated that porous Sn electrodes were more favorable to CO2 reduction in which it improved current density and had a more positive onset potential. Effects of concentration of KHCO3 and potential were investigated, which indicated the best catalytic activity existed in 0.5 mol/L KHCO3 electrolyte at -1.7 V vs.SCE, and the maximum current efficiency of formic acid reached 73.9%. Thus, porous electrode materials can effectively improve the catalytic effect of CO2 electroreduction.

Keywordsporous Sn electrode;   carbon dioxide;   electroreduction;   current density;   current efficiency     
Received 2014-05-20;
Fund:

国家自然科学基金(21206117)。

Corresponding Authors: 王华,E-mail: tjuwanghua@tju.edu.cn。     Email: tjuwanghua@tju.edu.cn
About author: 韩真真(1987-),女,硕士研究生,现从事电化学方面的研究。
引用本文:   
韩真真, 王华, 王静, 韩金玉.多孔锡电极的制备及其用于CO2电化学还原性能[J].  化学工业与工程, 2016,33(5): 8-13
Han Zhenzhen, Wang Hua, Wang Jing, Han Jinyu.Fabrication of Porous Tin and Its Application to Electroreduction of CO2[J].  Chemcial Industry and Engineering, 2016,33(5): 8-13
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