Fan Xiaokun, Chen Wen, Xie Lei, Liu Xianglong, Ding Yutian, Zhang Long, Tang Min, Liao Yujia, Yang Qi, Fu Xian-Zhu, Luo Shuiping, Luo Jing-Li
Bay Area Center for Electron Microscopy, Songshan Lake Materials Laboratory, Dongguan, 523808, P. R. China.
Department of Chemistry, Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Southern University of Science and Technology (SUSTech), Shenzhen, Guangdong, 518055, P. R. China.
Adv Mater. 2024 May;36(21):e2313179. doi: 10.1002/adma.202313179. Epub 2024 Feb 22.
Single-atom decorating of Pt emerges as a highly effective strategy to boost catalytic properties, which can trigger the most Pt active sites while blocking the smallest number of Pt atoms. However, the rational design and creation of high-density single-atoms on Pt surface remain as a huge challenge. Herein, a customized synthesis of surface-enriched single-Bi-atoms tailored Pt nanorings (SE-Bi/Pt NRs) toward methanol oxidation is reported, which is guided by the density functional theory (DFT) calculations suggesting that a relatively higher density of Bi species on Pt surface can ensure a CO-free pathway and accelerate the kinetics of *HCOOH formation. Decorating Pt NRs with dense single-Bi-atoms is achieved by starting from PtBi intermetallic nanoplates (NPs) with intrinsically isolated Bi atoms and subsequent etching and annealing treatments. The SE-Bi/Pt NRs exhibit a mass activity of 23.77 A mg Pt toward methanol oxidation in alkaline electrolyte, which is 2.2 and 12.8 times higher than those of Pt-Bi NRs and Pt/C, respectively. This excellent activity endows the SE-Bi/Pt NRs with a high likelihood to be used as a practical anodic electrocatalyst for direct methanol fuel cells （DMFCs） with high power density of 85.3 mW cm and ultralow Pt loading of 0.39 mg cm.
铂的单原子修饰成为提高催化性能的一种高效策略，它能激活最多的铂活性位点，同时阻断最少数量的铂原子。然而，在铂表面合理设计并制备高密度单原子仍然是一个巨大的挑战。在此，报道了一种针对甲醇氧化的表面富集单铋原子定制合成的铂纳米环（SE-Bi/Pt NRs），其由密度泛函理论（DFT）计算指导，表明铂表面相对较高密度的铋物种可确保无CO路径并加速*HCOOH形成的动力学。通过从具有本征孤立铋原子的PtBi金属间纳米板（NPs）开始，经过后续蚀刻和退火处理，实现了用密集的单铋原子修饰铂纳米环。SE-Bi/Pt NRs在碱性电解质中对甲醇氧化表现出23.77 A mg Pt的质量活性，分别是Pt-Bi NRs和Pt/C的2.2倍和12.8倍。这种优异的活性使SE-Bi/Pt NRs极有可能用作直接甲醇燃料电池（DMFCs）的实用阳极电催化剂，其具有85.3 mW cm的高功率密度和0.39 mg cm的超低铂负载量。
