物理化学学报 >> 2013, Vol. 29 >> Issue (05): 989-995.doi: 10.3866/PKU.WHXB201303121

电化学和新能源 上一篇    下一篇

Pt 纳米颗粒在聚二甲基二烯丙基氯化铵功能化碳纳米管上的自发沉积及其对甲醇的电氧化性能

崔颖1, 匡尹杰1,2, 张小华1, 刘博3, 陈金华1   

  1. 1 湖南大学化学化工学院, 化学生物传感与计量学国家重点实验室, 长沙 410082;
    2 长沙理工大学化学与生物工程学院, 电力与交通材料保护湖南省重点实验室, 长沙 410114;
    3 西北有色金属研究院, 西安泰金工业电化学技术有限公司, 西安 710016
  • 收稿日期:2012-12-17 修回日期:2013-03-11 发布日期:2013-04-24
  • 通讯作者: 刘博, 陈金华 E-mail:chenjinhua@hnu.edu.cn; net_lb@163.com
  • 基金资助:

    国家自然科学基金(21275041, 21235002, 21221003); 湖南省自然科学基金(12JJ2010)及高等学校博士学科点专项科研基金(20110161110009)资助项目

Spontaneous Deposition of Pt Nanoparticles on Poly(diallyldimethylammonium chloride)/Carbon Nanotube Hybrids and Their Electrocatalytic Oxidation of Methanol

CUI Ying1, KUANG Yin-Jie1,2, ZHANG Xiao-Hua1, LIU Bo3, CHEN Jin-Hua1   

  1. 1 State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, P. R. China;
    2 Hunan Provincial Key Laboratory of Materials Protection for Electric Power and Transportation, School of Chemistry and Biological Engineering, Changsha University of Science & Technology, Changsha, 410114, P.R. China;
    3 Xi’an Taijin Industrial Electrochemical Technology Co., Ltd, Northwest Institute For Non-ferrous Metal Research, Xi’an 710016, PR China
  • Received:2012-12-17 Revised:2013-03-11 Published:2013-04-24
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (2127504, 21235002, 21221003), Natural Science Foundation of Hunan Province, China (12JJ2010), and Specialized Research Fund for the Doctoral Program of Higher Education, China (20110161110009).

摘要:

利用聚二甲基二烯丙基氯化铵(PDDA)非共价修饰的碳纳米管(CNTs)与PtCl62-之间的自发氧化还原作用, 制备了Pt 纳米颗粒(Pt NPs)/CNTs-PDDA复合催化剂. PDDA在该催化剂中具有三种作用: (1) 作为金属前驱体PtCl62-还原为Pt NPs 的还原剂; (2) 作为原位产生的Pt NPs 的稳定剂; (3) 在CNTs 表面形成保护膜抑制CNTs 在甲醇电催化氧化过程中的腐蚀. 采用傅里叶变换红外(FTIR)光谱、热重分析和拉曼光谱对CNTs-PDDA进行了表征, 表明PDDA通过π-π作用已成功覆盖在CNTs 表面, 并且修饰过程没有导致CNTs 结构的破坏. 采用透射电子显微镜(TEM)对Pt NPs/CNTs-PDDA 催化剂进行了表征, 结果表明, Pt NPs 均匀地分散在CNTs上, 平均粒径约2 nm, 且粒径分布范围窄. 用循环伏安法、计时电流法进一步考察了Pt NPs/CNTs-PDDA催化剂在酸性介质中对甲醇的电催化氧化的性能. 电化学测试结果表明, 与原始CNTs 负载的Pt NPs催化剂相比,Pt NPs/CNTs-PDDA催化剂具有更高的电化学活性表面积、电催化质量比活性和稳定性.

关键词: Pt纳米颗粒, 甲醇, 电催化氧化, 聚二甲基二烯丙基氯化铵, 碳纳米管

Abstract:

Carbon nanotubes were non-covalently functionalized by poly(diallyldimethylammonium chloride) (PDDA). Here, PDDA has three roles: reductant for the metal precursor of PtCl62-, stabilizer for in-situ produced Pt nanoparticles (Pt NPs), and anti-corrosion film for carbon nanotubes (CNTs). Surface-functionalization of CNTs with PDDA was characterized by Fourier transform infrared (FTIR) spectrometry, thermogravimetric analysis, and Raman spectroscopy. The results indicated that the surface of CNTs was successfully coated with PDDA film by π-π stacking interactions, and the functionalization process had no detrimental effect on the structure of the CNTs. The obtained catalyst (Pt NPs/ CNTs-PDDA) was characterized by transmission electron microscopy, and the results showed that Pt NPs with an average diameter of ca 2 nm were highly dispersed on the surface of CNTs-PDDA. The electrocatalytic properties of Pt NPs/CNTs-PDDA nanohybrids for methanol oxidation were further characterized by cyclic voltammetry and chronoamperometry. Compared with Pt NPs supported on the pristine CNTs, the Pt NPs/CNTs-PDDA catalyst had higher electrochemical surface area and specific mass activity, and better stability towards methanol electro-oxidation.

Key words: Pt nanoparticle, Methanol, Electrocatalytic oxidation, PDDA, Carbon nanotube

MSC2000: 

  • O643