Yun Qinru, Xu Juan, Wei Tingcha, Ruan Qifeng, Zhu Xingzhong, Kan Caixia
College of Science, Nanjing University of Aeronautics and Astronautics, Nanjing 211106, China.
Key Laboratory of Aerospace Information Materials and Physics (NUAA), MIIT, Nanjing 211106, China.
Nanoscale. 2022 Jan 20;14(3):736-743. doi: 10.1039/d1nr05987d.
Au-Pd hollow nanostructures have attracted a lot of attention because of their excellent ethanol electrooxidation performance. Herein, we report a facile preparation of Au nanoframe@Pd array electrocatalysts in the presence of cetylpyridinium chloride. The reduced Pd atoms were directed to mainly deposit on the surface of the Au nanoframes in the form of rods, leading to the formation of Au nanoframe@Pd arrays with a super-large specific surface area. The red shift and damping of the plasmon peak were ascribed to the deposition of the Pd arrays on the surface of the Au nanoframes and nanobipyramids, which was verified by electrodynamic simulations. Surfactants, temperature and reaction time determine the growth process and thereby the architecture of the obtained Au-Pd hollow nanostructures. Compared with the Au nanoframe@Pd nanostructures and Au nanobipyramid@Pd arrays, the Au nanoframe@Pd arrays exhibit an enhanced electrocatalytic performance towards ethanol electrooxidation due to an abundance of catalytic active sites. The Au NF@Pd arrays display 4.1 times higher specific activity and 13.7 times higher mass activity than the commercial Pd/C electrocatalyst. Moreover, the nanostructure shows improved stability towards the ethanol oxidation reaction. This study enriches the manufacturing technology to increase the active sites of noble metal nanocatalysts and promotes the development of direct ethanol fuel cells.
金-钯中空纳米结构因其优异的乙醇电氧化性能而备受关注。在此,我们报道了在十六烷基吡啶氯化物存在下简便制备金纳米框架@钯阵列电催化剂的方法。还原后的钯原子主要以棒状形式沉积在金纳米框架表面,从而形成具有超大比表面积的金纳米框架@钯阵列。等离子体峰的红移和阻尼归因于钯阵列沉积在金纳米框架和纳米双锥体表面,这通过电动力学模拟得到了验证。表面活性剂、温度和反应时间决定了生长过程,进而决定了所得金-钯中空纳米结构的结构。与金纳米框架@钯纳米结构和金纳米双锥体@钯阵列相比,金纳米框架@钯阵列由于具有丰富的催化活性位点,对乙醇电氧化表现出增强的电催化性能。金纳米框架@钯阵列的比活性比商业钯/碳电催化剂高4.1倍,质量活性高13.7倍。此外,该纳米结构对乙醇氧化反应表现出更高的稳定性。这项研究丰富了增加贵金属纳米催化剂活性位点的制造技术,促进了直接乙醇燃料电池的发展。