Chen Ligang, Liang Xin, Wang Dingsheng, Yang Zuobo, He Chun-Ting, Zhao Wei, Pei Jiajing, Xue Yanrong
State Key Laboratory of Chemical Resource Engineering, Beijing Advanced Innovation Centre for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
State Power Investment Corporation Hydrogen Energy Company, Limited, Beijing 102209, China.
ACS Appl Mater Interfaces. 2022 Jun 22;14(24):27814-27822. doi: 10.1021/acsami.2c02905. Epub 2022 Jun 12.
The precise regulation for the structural properties of nanomaterials at the atomic scale is an effective strategy to develop high-performance catalysts. Herein, a facile dual-regulation approach was developed to successfully synthesize RuPt single atom alloy (SAA) with atomic Ru dispersed in Pt nanocrystals. High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure demonstrated that Ru atoms were dispersed in Pt nanocrystals as single atoms. Impressively, the RuPt-SAA exhibited an ultrahigh specific activity (23.59 mA cm) and mass activity (2.805 mA/μg) for methanol oxidation reaction (MOR) and exhibited excellent exchange current density activity (1.992 mA cm) and mass activity (4.71 mA/μg) for hydrogen oxidation reaction (HOR). Density functional theory calculations revealed that the introduction of Ru atoms greatly reduced the reaction free energy for the decomposition of water molecules, which promoted the removal of CO* in the MOR process and adjusted the Gibbs free energy of hydrogen and hydroxyl adsorption to promote the HOR. Our work provided an effective idea for the development of high performance electrocatalysts.
在原子尺度上精确调控纳米材料的结构性质是开发高性能催化剂的有效策略。在此,我们开发了一种简便的双调控方法,成功合成了RuPt单原子合金(SAA),其中Ru原子以单原子形式分散在Pt纳米晶体中。高角度环形暗场扫描透射电子显微镜和X射线吸收精细结构表明,Ru原子以单原子形式分散在Pt纳米晶体中。令人印象深刻的是,RuPt-SAA对甲醇氧化反应(MOR)表现出超高的比活性(23.59 mA cm)和质量活性(2.805 mA/μg),对氢氧化反应(HOR)表现出优异的交换电流密度活性(1.992 mA cm)和质量活性(4.71 mA/μg)。密度泛函理论计算表明,Ru原子的引入大大降低了水分子分解的反应自由能,促进了MOR过程中CO*的去除,并调整了氢和羟基吸附的吉布斯自由能以促进HOR。我们的工作为开发高性能电催化剂提供了一个有效的思路。