Li Junjie, Jiang Ya-Fei, Wang Qi, Xu Cong-Qiao, Wu Duojie, Banis Mohammad Norouzi, Adair Keegan R, Doyle-Davis Kieran, Meira Debora Motta, Finfrock Y Zou, Li Weihan, Zhang Lei, Sham Tsun-Kong, Li Ruying, Chen Ning, Gu Meng, Li Jun, Sun Xueliang
Department of Mechanical and Materials Engineering, University of Western Ontario, London, ON, N6A 5B9, Canada.
Department of Chemistry, Southern University of Science and Technology, 518055, Shenzhen, China.
Nat Commun. 2021 Nov 23;12(1):6806. doi: 10.1038/s41467-021-27143-5.
Single-atom catalysts (SACs) have been applied in many fields due to their superior catalytic performance. Because of the unique properties of the single-atom-site, using the single atoms as catalysts to synthesize SACs is promising. In this work, we have successfully achieved Co SAC using Pt atoms as catalysts. More importantly, this synthesis strategy can be extended to achieve Fe and Ni SACs as well. X-ray absorption spectroscopy (XAS) results demonstrate that the achieved Fe, Co, and Ni SACs are in a M-pyrrolic N (M= Fe, Co, and Ni) structure. Density functional theory (DFT) studies show that the Co(Cp) dissociation is enhanced by Pt atoms, thus leading to the formation of Co atoms instead of nanoparticles. These SACs are also evaluated under hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and the nature of active sites under HER are unveiled by the operando XAS studies. These new findings extend the application fields of SACs to catalytic fabrication methodology, which is promising for the rational design of advanced SACs.
单原子催化剂（SACs）因其卓越的催化性能已被应用于许多领域。由于单原子位点的独特性质，利用单原子作为催化剂来合成SACs具有广阔前景。在这项工作中，我们成功地以Pt原子作为催化剂实现了Co SAC的合成。更重要的是，这种合成策略也可以扩展用于制备Fe和Ni SACs。X射线吸收光谱（XAS）结果表明，所制备的Fe、Co和Ni SACs具有M-吡咯N（M = Fe、Co和Ni）结构。密度泛函理论（DFT）研究表明，Pt原子增强了Co(Cp)的解离，从而导致Co原子的形成而非纳米颗粒。这些SACs还在析氢反应（HER）和析氧反应（OER）条件下进行了评估，并且通过原位XAS研究揭示了HER条件下活性位点的本质。这些新发现将SACs的应用领域扩展到催化制备方法，这对于先进SACs的合理设计具有重要意义。
