二维碳载Au4Pd2催化剂的构建及其电催化性能

doi:10.19799/j.cnki.2095-4239.2021.0305

摘要/Abstract

摘要：

贵金属纳米团簇由于精确的结构和明确的化学组成而受到广泛的关注。该工作采用具有精准的颗粒大小和精确的结构双金属金属纳米团簇，研究其电子结构、几何结构对催化反应的影响，同时利用杂原子与主原子间的强电子耦合作用调控催化性能。首先制备4个金原子与2个钯原子组成的金钯纳米团簇，并分散至二维材料上得到单团簇分散的金钯基纳米复合材料催化剂；通过XPS测试可知，AuPd与载体之间存在较强的协同作用，有助于促进其氧还原(ORR)与析氢反应(HER)的稳定性；调节贵金属比例得到最佳比例的金钯催化剂，在0.1 mol/L KOH氧饱和电解液中，起始电位为0.95 V，半波电位为0.81 V，其ORR性能优于商业Pd/C。该催化剂也具有良好的HER性能，在0.5 mol/L H₂SO₄电解液中，电流密度为10 mA/cm²下的过电位为129 mV；利用X射线衍射(XRD)、X射线光电子能谱(XPS)、透射电镜(TEM)对催化剂结构进行表征分析，解释其结构与性能间的联系。优化贵金属团簇掺杂比例得到具有优异氧还原与析氢性能的双功能催化剂，为高效稳定的电催化剂的开发提供了新方向。

关键词: 贵金属团簇, 电催化剂, 金属空气电池, 氧还原, 氢析出

Abstract:

Noble metal nanoclusters have received widespread attention due to their special structure and distinct chemical composition. Bimetallic metal nanoclusters with precise particle size and structure were used in this study to investigate the effect of electronic and geometric structure on the catalytic reaction. The electron coupling between heteroatom and the host atom could regulate the catalytic performance. To create the well-dispersed electrochemical catalysts, carbon nanosheets supported Au₄Pd₂ nanoclusters (NCs) with a high surface area. The X-ray photoelectron spectroscopy (XPS) test revealed that the synergistic effect of AuPd and the support could promote ORR and HER stability. The ORR performance of Au₄Pd₂-CNs-2 with the initial potential of 0.95 V and the half-wave potential of 0.81 V was better than those of commercial Pd/C in the 0.1 mol/L KOH. The catalyst also demonstrated excellent catalytic activity towards HER with the overpotential of 129 mV at 10 mA/cm² in 0.5 mol/L H₂SO₄. The structure and morphology of catalysts are determined using X-ray diffraction (XRD) and transmission electron microscopy (TEM), and electrochemical measurements are used to test the electrocatalytic performances. Ultra-small single-cluster catalysts could improve the utilization and electrocatalytic activity of atoms, and the synergy effects between Au and Pd also enhance the catalytic activity of catalysts. By optimizing the doping ratio of Au₄Pd₂ NC_s, bifunctional catalysts with excellent oxygen reduction and hydrogen evolution performance were obtained, providing a new direction for developing non-platinum-based catalysts with high efficiency and stability.

Key words: noble metal nanoclusters, electrocatalysts, zinc-air batteries, oxygen reduction reaction, hydrogen evolution reaction

中图分类号:

TM 911

张申智, 王立开, 孙迎港, 吕恒, 杨子寅, 李磊磊, 李忠芳. 二维碳载Au₄Pd₂催化剂的构建及其电催化性能[J]. 储能科学与技术, 2021, 10(6): 2028-2038.

Shenzhi ZHANG, Likai WANG, Yinggang SUN, Heng LÜ, Ziyin YANG, Leilei LI, Zhongfang LI. Construction of two dimensional carbon-supported Au₄Pd₂ catalysts and their electrocatalytic performances[J]. Energy Storage Science and Technology, 2021, 10(6): 2028-2038.

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二维碳载Au₄Pd₂催化剂的构建及其电催化性能

Construction of two dimensional carbon-supported Au₄Pd₂ catalysts and their electrocatalytic performances

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