Chen Dong, Ye Feng, Liu Hui, Yang Jun
State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
University of Chinese Academy of Sciences, No. 19A Yuquan Road, Beijing 100049, China.
Sci Rep. 2016 Apr 15;6:24600. doi: 10.1038/srep24600.
Precisely tailoring the structure and fully making use of the components of nanoparticles are effective to enhance their catalytic performance for a given reaction. We herein demonstrate the design of cage-bell structured Pt-Pd nanoparticles, where a Pd shell is deliberately selected to enhance the catalytic property and methanol tolerance of Pt for oxygen reduction reaction. This strategy starts with the synthesis of core-shell Pt@Ag nanoparticles, followed by galvanic replacement reaction between the Ag shell and Pd(2+) ions to form core-shell-shell Pt@Ag@Ag-Pd nanoparticles with a Pt core and double shells composed of Ag at inner and alloy Ag-Pd at outer, respectively. Then, the core-shell-shell templates are agitated with saturated NaCl solution to eliminate the Ag component from the double shells, leading to the formation of bimetallic Pt-Pd nanoparticles with a cage-bell structure, defined as a movable Pt core enclosed by a porous Pd shell, which show enhanced catalytic activity for oxygen reduction compared with that of the Pt seeds due to the additional catalysis from Pd shell. In addition, owing to the different diffusion behavior of methanol and oxygen molecules in the porous Pd shell, the Pt-Pd cage-bell nanostructures also exhibit superior methanol tolerant property in catalyzing the oxygen reduction.
精确调整纳米颗粒的结构并充分利用其组成部分,对于增强其在特定反应中的催化性能是有效的。我们在此展示了笼钟结构的Pt-Pd纳米颗粒的设计,其中特意选择了Pd壳层以增强Pt对氧还原反应的催化性能和甲醇耐受性。该策略始于核壳结构的Pt@Ag纳米颗粒的合成,随后是Ag壳层与Pd(2+)离子之间的电化置换反应,以形成具有Pt核以及分别由内部的Ag和外部的合金Ag-Pd组成的双壳层的核壳壳层结构的Pt@Ag@Ag-Pd纳米颗粒。然后,将核壳壳层模板与饱和NaCl溶液搅拌以从双壳层中去除Ag组分,从而形成具有笼钟结构的双金属Pt-Pd纳米颗粒,其定义为由多孔Pd壳层包围的可移动Pt核,与Pt种子相比,由于Pd壳层的额外催化作用,其对氧还原表现出增强的催化活性。此外,由于甲醇和氧分子在多孔Pd壳层中的扩散行为不同,Pt-Pd笼钟纳米结构在催化氧还原时也表现出优异的甲醇耐受性。