物理化学学报 >> 2015, Vol. 31 >> Issue (9): 1727-1732.doi: 10.3866/PKU.WHXB201507161

电化学和新能源 上一篇    下一篇

PDDA修饰的碳纳米管载铂电催化剂的合成及其在碱性条件下的氧气还原反应催化性能

张杰,窦美玲,王峰*(),刘景军,李志林,吉静,宋夜   

  • 收稿日期:2015-05-06 发布日期:2015-09-06
  • 通讯作者: 王峰 E-mail:wangf@mail.buct.edu.cn
  • 基金资助:
    国家自然科学基金(51125007)

Synthesis of PDDA-Decorating MWCNTs Supported Pt Electrocatalysts and Catalytic Properties for Oxygen Reduction Reaction in Alkaline Medium

Jie. ZHANG,Mei-Ling. DOU,Feng. WANG*(),Jing-Jun. LIU,Zhi-Lin. LI,Jing. JI,Ye. SONG   

  • Received:2015-05-06 Published:2015-09-06
  • Contact: Feng. WANG E-mail:wangf@mail.buct.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(51125007)

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摘要：

采用长链聚合物聚二烯丙基二甲基氯化铵(PDDA)对多壁碳纳米管(MWCNTs)进行修饰,并将采用胶体法还原出的铂(Pt)纳米粒子通过静电作用担载于PDDA修饰的多壁碳纳米管上,从而制备出Pt/PDDA/MWCNTs复合电催化剂.透射电镜(TEM)与X射线衍射(XRD)测试结果表明, Pt纳米粒子均匀地分布在MWCNTs的表面,其平均粒径约为3.6 nm.热失重分析显示催化剂的实际负载量为36%(w).旋转圆盘电极测试结果表明, Pt/PDDA/MWCNTs催化剂对碱性条件下的氧气还原反应(ORR)具有优异的催化活性.与负载量为40%(w)的商业Pt/C催化剂相比, Pt/PDDA/MWCNTs催化剂的氧气还原反应的起始电位和半波电位均正移约30 mV,其质量比活性更大.动力学研究结果进一步证实Pt/PDDA/MWCNTs催化剂比负载量为40%(w)的商业Pt/C催化剂在碱性条件下对氧气还原反应具有更优异的催化活性.

关键词: 铂, 聚二烯丙基二甲基氯化铵, 多壁碳纳米管, 氧气还原反应

Abstract:

Multi-walled carbon nanotubes (MWCNTs) were modified with the long-chain polymer poly (diallyldimethylammonium chloride) (PDDA) and used as support for Pt nanoparticles (NPs). Pt/PDDA/ MWCNTs electrocatalysts were prepared by electrostatic adsorption of Pt NPs on the PDDA/MWCNTs support. Transmission electron microscopy (TEM) and X-ray diffraction (XRD) characterization revealed that the Pt NPs were well dispersed on the PDDA/MWCNTs support, with an average diameter of ~3.6 nm. Thermo gravimetric analysis showed that the loading of Pt was 36%(w). Rotating disk electrode (RDE) measurements showed that the Pt/PDDA/MWCNTs catalyst had excellent electrocatalytic activity for oxygen reduction in alkaline medium. Compared with commercial Pt/C (40%(w)), the Pt/PDDA/MWCNTs catalyst exhibited a positive shift of 30 mV for the oxygen reduction onset and half-wave potential. Kinetics study further confirmed the significantly enhanced oxygen reduction activity of the Pt/PDDA/MWCNTs catalyst in the alkaline medium.

Key words: Platinum, Poly(diallyldimethylammonium chloride), Multi-walled carbon nanotubes, Oxygen reduction reaction