Xu Yurui, Liu Xiao, Jiang Minghui, Chi Bichuan, Lu Yue, Guo Jin, Wang Ziming, Cui Suping
College of Materials Science & Engineering, Beijing University of Technology, Beijing 100124, China; Institute of Disaster Prevention, Sanhe 065201, China.
College of Materials Science & Engineering, Beijing University of Technology, Beijing 100124, China.
J Colloid Interface Sci. 2024 Jul;665:365-375. doi: 10.1016/j.jcis.2024.03.137. Epub 2024 Mar 26.
Exploring highly selective and stable electrocatalysts is of great significance for the electrochemical conversion of CO into fuel. Herein, a three-dimensional (3D) nanostructure catalyst was developed by doping Pb single-atom (Pb) in-situ on carbon paper (Pb-Cu/CP) through a low-energy and economical method. The designed catalyst exhibited abundant active sites and was beneficial to CO adsorption, activation, and subsequent conversion to fuel. Interestingly, Pb-Cu/CP showed a prominent Faraday efficiency (FE) of 97 % at -0.9 V versus reversible hydrogen electrode (vs. RHE) and a high partial current density of 27.9 mA·cm for formate. Also, the catalyst remained significantly stable for 60 h during the durability test. The reaction mechanism was investigated by density functional theory (DFT), demonstrating that the doping Pb induced the electrons redistribution, promoted the formate generation, reduced the rate-determining step (RDS) energy barrier, and inhibited the hydrogen evolution reaction. The study aims to provide a new strategy for developing of single-atom catalysts with high selectivity and stability, which will help reduce environmental pressure and alleviate energy problems.
探索高选择性和稳定性的电催化剂对于将CO电化学转化为燃料具有重要意义。在此，通过一种低能量且经济的方法，在碳纸上原位掺杂Pb单原子（Pb），制备了一种三维（3D）纳米结构催化剂（Pb-Cu/CP）。所设计的催化剂具有丰富的活性位点，有利于CO的吸附、活化以及随后转化为燃料。有趣的是，相对于可逆氢电极（vs. RHE），Pb-Cu/CP在-0.9 V时表现出97%的显著法拉第效率（FE），并且甲酸盐的高部分电流密度为27.9 mA·cm 。此外，在耐久性测试期间，该催化剂在60小时内保持显著稳定。通过密度泛函理论（DFT）研究了反应机理，结果表明掺杂的Pb引起电子重新分布，促进了甲酸盐的生成，降低了速率决定步骤（RDS）的能垒，并抑制了析氢反应。该研究旨在为开发具有高选择性和稳定性的单原子催化剂提供一种新策略，这将有助于减轻环境压力并缓解能源问题。
