Wang Sihao, Xu Wei, Zhu Yingfang, Luo Qingyu, Zhang Cheng, Tang Shaolong, Du Youwei
Jiangsu Key Laboratory for Nanotechnology, Collaborative Innovation Center of Advanced Microstructures, Nanjing National Laboratory of Microstructures, Department of Physics, Nanjing University, Nanjing 210093, P. R. China.
Fujian Provincial Key Laboratory of Functional Marine Sensing Materials, College of Physics and Electronic Information Engineering, Minjiang University, Fuzhou 350108, P. R. China.
ACS Appl Mater Interfaces. 2021 Jan 13;13(1):827-835. doi: 10.1021/acsami.0c21348. Epub 2020 Dec 28.
Constructing robust and cost-effective Pt-based electrocatalysts with an easily operated strategy remains a crucial obstacle to fuel cell applications. Conventional Pt-based catalysts suffer from high Pt content and an arduous synthetic process. Herein, through the spray dehydration method and annealing treatment, facile producible synthesis of a small-sized (5.2 nm) low-Pt (10.5 wt %) ordered PtCo/C catalyst (O-PtCo/C) for oxygen reduction reaction is reported. The fast spray evaporation rate contributes to small size and uniform nucleation of nanoparticles (NPs) on carbon support. O-PtCo/C-600 exhibits efficient electrocatalytic performance with mass activity (MA) 6.0-fold and specific activity 3.9-fold higher than commercial Pt/C. The ordered chemical structure generates superior stability with merely 3.5% decay in MA after 10,000 potential cycles. Density functional theory calculations reveal that the enhanced catalytic performance originates from rational modification of d-band through strain and ordering effect and accompanying weaker adsorption of intermediate OH. This work highlights the potentials of low-Pt PtM-type ordered NPs for prospective fuel cell cathodic catalysis. The proposed facile and practical synthetic strategy also shows promising prospects for preparing effective Pt-based electrocatalysts.
采用易于操作的策略构建坚固且经济高效的铂基电催化剂仍然是燃料电池应用的关键障碍。传统的铂基催化剂存在铂含量高和合成过程艰巨的问题。在此，通过喷雾干燥法和退火处理，报道了一种易于制备的用于氧还原反应的小尺寸（5.2纳米）低铂（10.5重量%）有序铂钴/碳催化剂（O-PtCo/C）。快速的喷雾蒸发速率有助于在碳载体上形成小尺寸且均匀成核的纳米颗粒（NPs）。O-PtCo/C-600表现出高效的电催化性能，其质量活性（MA）比商业铂/碳高6.0倍，比活性高3.9倍。有序的化学结构产生了优异的稳定性，在10000次电位循环后MA仅衰减3.5%。密度泛函理论计算表明，催化性能的增强源于通过应变和有序效应合理修饰d带以及随之而来的中间体OH吸附减弱。这项工作突出了低铂PtM型有序NPs在未来燃料电池阴极催化方面的潜力。所提出的简便实用的合成策略在制备有效的铂基电催化剂方面也显示出广阔的前景。
