高等学校化学学报 ›› 2018, Vol. 39 ›› Issue (1): 157-165.doi: 10.7503/cjcu20170168

• 物理化学 • 上一篇    下一篇

Pt-CeO2/聚苯乙烯磺酸盐功能化碳纳米管复合物的制备及对甲醇的电催化氧化性能

陈晨, 李丽, 陈金华(), 张小华(), 许杰, 李益波, 韦杰   

  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
  • 收稿日期:2017-03-22 出版日期:2018-01-10 发布日期:2017-12-19
  • 作者简介:联系人简介: 张小华, 女, 博士, 副教授, 主要从事表面处理及高分子材料研究. E-mail:mickyxie@hnu.edu.cn; 陈金华, 男, 博士, 教授, 主要从事纳米材料和电催化材料研究. E-mail:chenjinhua@hnu.cn
  • 基金资助:
    国家自然科学基金(批准号: 21475035, 21235002, 21275041)、 长江学者和创新团队发展计划项目(批准号: PCSIRT)、 湖南省自然科学基金(批准号:12JJ2010)、 国家自然科学基金创新研究群体基金(批准号: 21521063)和湖南大学大学生创新训练项目资助

Preparation and Electrocatalytic Performance for Methanol Oxidation of Pt-CeO2/Sodium-4-styrenesulfonate Functionalized Carbon Nanotube Composites

CHEN Chen, LI Li, CHEN Jinhua*(), ZHANG Xiaohua*(), XU Jie, LI Yibo, WEI Jie   

  1. State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, China
  • Received:2017-03-22 Online:2018-01-10 Published:2017-12-19
  • Contact: CHEN Jinhua,ZHANG Xiaohua E-mail:chenjinhua@hnu.cn;mickyxie@hnu.edu.cn
  • Supported by:
    † Supported by the National Natural Science Foundation of China(Nos.21475035, 21235002, 21275041), the Program for Changjiang Scholars and Innovative Research Team in University, China(No.PCSIRT), the Hunan Provincial Natural Science Fund, China(No.12JJ2010), the Science Fund for Creative Research Groups of the National Natural Science Foundation of China(No.21521063) and the Students Innovation Training Program at Hunan University, China

摘要:

通过阴离子聚合物聚苯乙烯磺酸钠(PSS)对碳纳米管(CNTs)进行非共价功能化修饰得到PSS 功能化的碳纳米管(PSS-CNTs), 利用带负电的PSS和Ce3+之间的静电作用将Ce3+组装到CNTs表面, 再利用Ce3+与PtCl42-之间存在的静电作用和氧化还原反应实现CeO2和Pt纳米粒子在CNTs表面的原位沉积, 得到复合催化剂Pt-CeO2/PSS-CNTs. 采用透射电子显微镜(TEM)、 X射线衍射仪(XRD)、 能谱仪(EDS)及拉曼光谱仪(Raman)等对催化剂进行了表征. 电化学性能测试结果表明, 由于PSS-CNTs表面原位沉积的Pt纳米粒子相对于在原始CNTs上沉积的Pt纳米粒子具有更小的粒径、 更好的分散均匀性和稳定性, 同时Pt与CeO2之间存在良好的协同效应, Pt-CeO2/PSS-CNTs催化剂对甲醇电催化氧化具有较好的催化活性和化学稳定性, 当nPt/nCe=2/3时催化性能最优.

关键词: 直接甲醇燃料电池, 功能化碳纳米管, 稀土氧化物, 电催化活性, 稳定性

Abstract:

Carbon nanotubes(CNTs) were noncovalently modified by anionic polymer poly(sodium-4-styrenesulfonate)(PSS) to obtain PSS functionalized CNTs(PSS-CNTs), and then Ce3+ was assembled to CNTs surface through the electrostatic interaction between electropositive Ce3+ and electronegative PSS. Through the electrostatic interaction and oxidation-reduction reaction between Ce3+and PtCl42-, CeO2 and Pt nanoparticles were in-situ deposited on the surface of CNTs to obtain PSS-CNTs supported Pt-CeO2 composite catalyst(Pt-CeO2/PSS-CNTs). The structure, component and micromorphology of Pt-CeO2/PSS-CNTs were characterized by transmission electron microscopy(TEM), X-ray diffraction(XRD), X ray photoelectron spectroscopy(XPS), energy dispersive X-ray spectroscopy(EDS) and Raman spectroscopy, respectively. The electrochemical study shows that, due to the smaller particle size, the better dispersion uniformity and stability of Pt nanoparticles in-situ deposited on the surface of PSS-CNTs compared with those on the original CNTs, and the synergetic effect between Pt and CeO2, Pt-CeO2/PSS-CNTs, especially Pt-CeO2/PSS-CNTs with nPt/nCe of 2/3, exhibits higher catalytic activity and stability for methanol electrooxidation compared with Pt-CeO2/CNTs and PtRu/C.

Key words: Direct methanol fuel cell, Functionalized carbon nanotubes, Rare earth oxide, Electrocatalytic activity, Stability

中图分类号: