物理化学学报 >> 2014, Vol. 30 >> Issue (4): 708-714.doi: 10.3866/PKU.WHXB201401222

催化和表面科学 上一篇    下一篇

过生长法制备准凹面体状Pt-Ni纳米合金及其甲醇氧化电催化性能

王纯, 康建新, 王利利, 陈庭文, 李杰, 张东凤, 郭林   

  1. 仿生智能界面科学与技术教育部重点实验室, 仿生能源材料与器件北京市重点实验室,北京航空航天大学化学与环境学院, 北京100191
  • 收稿日期:2013-12-03 修回日期:2014-01-21 发布日期:2014-03-31
  • 通讯作者: 张东凤, 郭林 E-mail:dfzhang@buaa.edu.cn;guolin@buaa.edu.cn
  • 基金资助:

    国家自然科学基金(21173015)及国家重点基础研究发展规划项目(973)(2010CB934700)资助

Synthesis of Quasi-Concave Pt-Ni Nanoalloys via Overgrowth and Their Catalytic Performance towards Methanol Oxidation

WANG Chun, KANG Jian-Xin, WANG Li-Li, CHEN Ting-Wen, LI Jie, ZHANG Dong-Feng, GUO Lin   

  1. Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, Beijing Key Laboratory of Bio-inspired Energy Materials and Devices, School of Chemistry and Environment, Beihang University, Beijing 100191, P. R. China
  • Received:2013-12-03 Revised:2014-01-21 Published:2014-03-31
  • Contact: ZHANG Dong-Feng, GUO Lin E-mail:dfzhang@buaa.edu.cn;guolin@buaa.edu.cn
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (21173015) and National Key Basic Research Program of China (973) (2010CB934700).

摘要:

通过溶剂热法,成功制备了准凹面体状Pt-Ni合金纳米结构. 不同角度的透射电镜照片和三维模型图表明,准凹面体与以立方八面体为基底,在其十二个顶点进行外延生长所形成的结构相对应. 高分辨电镜(HRTEM),选区电子衍射(SAED)和X射线粉末衍射(XRD)表征结果表明,外延部分与内核部分组成成分不同. 在进行系统对照实验的基础上提出了同步刻蚀-过生长机理来解释准凹面体的形成过程. 电化学测试表明,准凹面体对甲醇氧化具有很高的催化活性,按质量归一的催化活性是相同条件下制备所得纯Pt 颗粒的3 倍,是商用Pt/C 的13.6倍. X射线光电子能谱数据表明,Ni 的引入有效降低了Pt 的原子结合能,这可能对催化活性的提高起到了关键作用.

关键词: 过生长法, 准凹面体, Pt-Ni, 甲醇氧化反应, 电催化

Abstract:

Quasi-concave Pt-Ni alloy nanostructures were synthesized via a solvothermal method, and were thought to form by epitaxial growth on the 12 vertexes of a cuboctahedron. A simultaneous etchingovergrowth process was proposed to illustrate the growth mechanism. The epitaxial layer was of different composition from the core, as confirmed by high-resolution transmission electron microscopy, selectedarea electron diffraction and powder X-ray diffraction characterizations. The concave structures exhibited high catalytic activity towards methanol oxidation. The mass-normalized catalytic activity of the concave products was ~3 times that of pure Pt nanoparticles synthesized under similar conditions, and 13.6 times that of commercial Pt/C. X-ray photoelectron spectroscopy characterization indicated that the binding energy of the concave structures shifted to lower energy, relative to the pure Pt. The modified electronic structure by introducing Ni was thought to be responsible for the enhanced catalytic activity.

Key words: Overgrowth, Quasi-concave, Pt-Ni, Methanol oxidation reaction, Electrocatalysis

MSC2000: 

  • O643