物理化学学报 >> 2013, Vol. 29 >> Issue (01): 144-150.doi: 10.3866/PKU.WHXB201210092

催化和表面科学 上一篇    下一篇

EDTA对活性炭的功能化处理及其对炭载Pd催化剂电催化性能的影响

曹剑瑜1,2, 汤佳丽1, 宋玲政1, 许娟1,2, 王文昌1,2, 陈智栋1,2,3   

  1. 1 常州大学石油化工学院, 江苏常州 213164;
    2 江苏省太阳能电池与储能技术重点实验室, 江苏常州 213164;
    3 日本阔智电子有限公司, 日本大阪 590-0906
  • 收稿日期:2012-07-16 修回日期:2012-10-08 发布日期:2012-12-14
  • 通讯作者: 陈智栋 E-mail:zdchen.lab@gmail.com
  • 基金资助:

    国家自然科学基金(21003015, 21103014); 江苏省自然科学基金(BE201113, 2011Z0062)和江苏高校优势学科建设工程(PAPD)资助项目

Functionalization of Activated Carbon with EDTA and Its Effect on Electrocatalytic Performance of Carbon Supported Pd Catalysts

CAO Jian-Yu1,2, TANG Jia-Li1, SONG Ling-Zheng1, XU Juan1,2, WANG Wen-Chang1,2, Chen Zhi-Dong1,2,3   

  1. 1 School of Petrochemical Engineering, Changzhou University, Changzhou 213164, Jiangsu Province, P. R. China;
    2 Key Laboratory for Solar Cells and Energy Storage Technology of Jiangsu Province, Changzhou 213164, Jiangsu Province, P. R. China;
    3 Qualtec Co. Ltd., Osaka 590-0906, Japan
  • Received:2012-07-16 Revised:2012-10-08 Published:2012-12-14
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21003015, 21103014), Natural Science Foundation of Jiangsu Province, China (BE201113, 2011Z0062), and Project Funded by the Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions, China.

摘要:

采用乙二胺四乙酸(EDTA)对活性炭进行功能化处理, 研究了其对表面基团、炭载Pd 纳米粒子结构及Pd催化剂电催化性能的影响. 傅里叶变换红外(FTIR)光谱和X射线光电子能谱(XPS)表征表明, EDTA处理在炭表面引入了含氮基团. X射线粉末衍射(XRD)光谱、透射电镜(TEM)和电化学测试结果显示, 活性炭经EDTA处理后, 负载的Pd粒子粒径虽有所增大, 但由于炭载体与Pd粒子相互作用的增强, Pd利用率增加, 催化剂对甲酸氧化的活性和稳定性均显著提高. 电化学阻抗谱(EIS)分析进一步揭示, 甲酸在该催化剂电极上的电氧化反应具有较低的电荷传递电阻.

关键词: 炭载钯催化剂, 乙二胺四乙酸, 电催化, 甲酸氧化, 电化学阻抗谱

Abstract:

The effect of functionalization of activated carbon with ethylenediamine tetraacetic acid (EDTA) on surface functional groups, the structure of carbon-supported Pd nanoparticles, and the electrocatalytic performance of Pd catalysts were investigated. Fourier transform infrared (FTIR) spectroscopy and X-ray photoelectron spectroscopy (XPS) indicate that N-containing groups are introduced to the carbon surface via EDTA treatment. X-ray powder diffraction (XRD) spectra, transmission electron microscopy (TEM), and electrochemical measurements demonstrate that the electrocatalytic activity and stability for carbon-supported Pd catalysts were substantially enhanced when the carbon support was treated with EDTA, although the Pd particles size increased slightly. The improved electrocatalytic performance may be due to enhanced interactions between the Pd particles and the carbon support, resulting in an improved Pd utilization. Electrochemical impedance spectrum analysis further reveals that the Pd catalyst on EDTA-treated carbon (Pd/C-E) displayed a lower charge-transfer resistance for the electro-oxidation reaction of formic acid.

Key words: Carbon supported palladium catalyst, Ethylenediamine tetraacetic acid, Electrocatalysis, Formic acid oxidation, Electrochemical impedance spectrum

MSC2000: 

  • O646