磷酸钠水溶液中氧化还原循环制备三维银电极还原CO2生成CO

doi:10.11949/j.issn.0438-1157.20170797

化工学报 ›› 2017, Vol. 68 ›› Issue (12): 4809-4815.DOI: 10.11949/j.issn.0438-1157.20170797

• 材料化学工程与纳米技术 • 上一篇下一篇

磷酸钠水溶液中氧化还原循环制备三维银电极还原CO₂生成CO

何志桥, 魏榕飞, 严婷婷, 许旭杨, 陈建孟, 宋爽

浙江工业大学环境学院, 浙江杭州 310032

收稿日期:2017-06-22 修回日期:2017-08-30 出版日期:2017-12-05 发布日期:2017-12-05
通讯作者: 宋爽
基金资助:
国家自然科学基金项目（21477117，21177115）；浙江省自然科学基金杰出青年项目（LR14E080001）。

Preparation of three-dimensional Ag electrode by oxidation-reduction cycle method in sodium phosphate aqueous solution for reduction CO₂ to CO

HE Zhiqiao, WEI Rongfei, YAN Tingting, XU Xuyang, CHEN Jianmeng, SONG Shuang

College of Environment, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China

Received:2017-06-22 Revised:2017-08-30 Online:2017-12-05 Published:2017-12-05
Supported by:
supported by the National Natural Science Foundation of China (21477117, 21177115) and the Natural Science Foundation of Zhejiang Province (LR14E080001).

摘要/Abstract

摘要：

通过氧化还原循环制备了具有三维表面的纳米银电极（3D-Ag）。采用X射线衍射（XRD），场发射扫描电子显微镜（FE-SEM），高分辨透射电子显微镜（HRTEM）和双电位阶跃等方法研究了电极的结构和性能。制备的3D-Ag电极表面均匀分布了（100）和（111）晶面暴露的纳米Ag颗粒，颗粒直径为30～150 nm。通过CO₂的电催化还原实验考察了电极的催化活性和寿命，结果显示，相比未改性Ag片，改性3D-Ag电极具有更高的活性、选择性和稳定性。此外，3D-Ag电极在3组连续的2 h电还原CO₂实验中能保持较高活性，而未改性Ag电极随时间逐渐失去活性。3D-Ag电极表现出的高活性可归因于Ag纳米颗粒有利于*COOH的稳定化和吸附态还原中间体*CO的脱附。

关键词: Ag电极, 电化学, 纳米结构, 二氧化碳, 还原, 一氧化碳, 循环伏安

Abstract:

Silver electrode with a three-dimensional surface (3D-Ag) was synthesized by a facile oxidation-reduction cycle method. The structure and properties of the electrode were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), high-resolution transmission electron microscopy (HRTEM) and potential steps. The results showed that Ag nanoparticles with {100} and {111} facets exposed and a diameter of 30-150 nm dispersed uniformly on the as-prepared 3D-Ag. In comparison to untreated Ag plate, the synthesized 3D-Ag electrode exhibits superior activity, selectivity and stability toward electrocatalytic reduction of CO₂ to CO. Moreover, the 3D-Ag electrode could maintain its high activity during three successive periods of two hours, while the bulk silver electrode gradually lost its activity. The high performance of 3D-Ag electrode could be ascribed to that the Ag nanoparticles are beneficial to the stabilization of the surface adsorbed COOH species, and to the desorption of the reduction intermediates of adsorbed CO species during the reduction of CO₂.

Key words: silver electrode, electrochemistry, nanostructure, carbon dioxide, reduction, carbon monoxide, cyclic voltammetry

中图分类号:

O643

何志桥, 魏榕飞, 严婷婷, 许旭杨, 陈建孟, 宋爽. 磷酸钠水溶液中氧化还原循环制备三维银电极还原CO₂生成CO[J]. 化工学报, 2017, 68(12): 4809-4815.

HE Zhiqiao, WEI Rongfei, YAN Tingting, XU Xuyang, CHEN Jianmeng, SONG Shuang. Preparation of three-dimensional Ag electrode by oxidation-reduction cycle method in sodium phosphate aqueous solution for reduction CO₂ to CO[J]. CIESC Journal, 2017, 68(12): 4809-4815.

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磷酸钠水溶液中氧化还原循环制备三维银电极还原CO₂生成CO

Preparation of three-dimensional Ag electrode by oxidation-reduction cycle method in sodium phosphate aqueous solution for reduction CO₂ to CO

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