物理化学学报 >> 2017, Vol. 33 >> Issue (8): 1628-1634.doi: 10.3866/PKU.WHXB201704242

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石墨烯负载PtPd纳米催化剂的合成及其电催化氧化甲醇性能

杨翼1,罗来明1,陈迪2,刘洪鸣1,张荣华1,代忠旭2,*(),周新文1,*()   

  1. 1 三峡大学生物与制药学院,湖北宜昌443002
    2 三峡大学材料与化工学院,湖北宜昌443002
  • 收稿日期:2017-02-23 发布日期:2017-06-14
  • 通讯作者: 代忠旭,周新文 E-mail:Daizx@ctgu.edu.cn;xwzhou@ctgu.edu.cn
  • 基金资助:
    国家自然科学基金(21403126);国家自然科学基金(21503120);三峡大学培优基金(2016PY074)

Synthesis and Electrocatalytic Properties of PtPd Nanocatalysts Supported on Graphene for Methanol Oxidation

Yi YANG1,Lai-Ming LUO1,Di CHEN2,Hong-Ming LIU1,Rong-Hua ZHANG1,Zhong-Xu DAI2,*(),Xin-Wen ZHOU1,*()   

  1. 1 College of Biological and Pharmaceutical Science, China Three Gorges University, Yichang 443002, Hubei Province, P. R. China
    2 College of Materials and Chemical Engineering, China Three Gorges University, Yichang 443002, Hubei Province, P. R. China
  • Received:2017-02-23 Published:2017-06-14
  • Contact: Zhong-Xu DAI,Xin-Wen ZHOU E-mail:Daizx@ctgu.edu.cn;xwzhou@ctgu.edu.cn
  • Supported by:
    the National Natural Science Foundation of China(21403126);the National Natural Science Foundation of China(21503120);Startup Foundation from China Three Gorges University(2016PY074)

摘要:

采用改进的Hummers法制备氧化石墨烯,然后以其为载体前驱体,以三嵌段共聚物P123为还原剂、保护剂和形貌控制剂,分别采用液相共还原法和连续还原法,制备了三种石墨烯负载PtPd(PtPd/G)纳米催化剂;氧化石墨烯与金属前驱体同步还原,从而达到原位负载的效果。采用X射线衍射(XRD)、透射电镜(TEM)、X射线光电子能谱(XPS)等表征方法分析了PtPd/G纳米催化剂的形貌、结构和组成,结果表明:采用共还原法得到的两种催化剂均为纳米枝结构;采用连续还原法得到了空心纳米结构。电化学循环伏安法和计时电流法研究表明:空心结构PtPd/G纳米催化剂抗CO中毒能力最强,100℃下共还原合成的PtPd/G纳米枝催化剂具有最佳的电催化氧化甲醇性能,约是商业化Pt/C催化剂的1.5倍。

关键词: 石墨烯, 原位负载, 纳米枝, 空心结构, 甲醇氧化

Abstract:

This work describes the preparation of three kinds of PtPd/graphene (PtPd/G) nanocatalysts. Graphene oxide was first prepared as the carrier precursor by the Hummers method, and subsequently, the simultaneous reduction of graphene oxide and the metal precursor led to the in situ loading of PtPd on graphene. The fabrication procedure involving liquid phase co-reduction and successive reduction methods utilized the block copolymer P123 as a reducing agent, stabilizer, and morphology control agent. The morphology, structure, and composition of the obtained catalysts were studied by X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). It was found that the catalysts synthesized by the co-reduction method possess a nanodendritic structure, while those prepared by successive reduction exhibit a hollow structure. Cyclic voltammetry and chronoamperometry investigations revealed that the PtPd/G catalyst with a hollow structure displayed the best anti-CO poisoning properties. In contrast, the catalyst with a dendritic structure that had been prepared at 100℃ showed the highest electrocatalytic performance towards methanol oxidation, which was 1.5 times that of the commercial Pt/C electrocatalyst.

Key words: Graphene, In situ loading, Nanodendritic, Hollow structure, Methanol oxidation