Allasia Nicolò, Xu Shuai, Jafri Sadaf Fatima, Borfecchia Elisa, Cipriano Luis A, Terraneo Giancarlo, Tosoni Sergio, Mino Lorenzo, Di Liberto Giovanni, Pacchioni Gianfranco, Vilé Gianvito
Department of Chemistry, Materials and Chemical Engineering "Giulio Natta", Politecnico di Milano, Piazza Leonardo da Vinci 32, Milano, 20133, Italy.
Department of Materials Science, Università degli Studi di Milano-Bicocca, Via Roberto Cozzi 55, Milano, 20125, Italy.
Small. 2025 Jun;21(23):e2408286. doi: 10.1002/smll.202408286. Epub 2025 Jan 9.
Single-atom catalysts (SACs) are gathering significant attention in chemistry due to their unique properties, offering uniform active site distribution and enhanced selectivity. However, their precise structure often remains unclear, with multiple models proposed in the literature. Understanding the coordination environment of the active site at the atomic level is crucial for explaining catalytic activity. Here, a comprehensive study of SACs made of carbon nitride (CN) containing isolated nickel atoms is presented. Using a combination of synthesis techniques and characterization methods including Fourier-transform infrared spectroscopy, X-ray absorption spectroscopy (XAS), and density functional theory (DFT) calculations, the local environment of nickel active centers in CN-supported SACs is investigated. These results challenge conventional structural models and propose a new architecture that better aligns with current experimental evidence. This new structure serves as a foundational step toward a rational approach to catalyst development and can facilitate more precise design and application of these innovative catalysts.
单原子催化剂（SACs）因其独特的性质在化学领域备受关注，它具有均匀的活性位点分布并能提高选择性。然而，其精确结构往往仍不明确，文献中提出了多种模型。在原子水平上理解活性位点的配位环境对于解释催化活性至关重要。在此，本文对含孤立镍原子的氮化碳（CN）制成的单原子催化剂进行了全面研究。通过结合合成技术和表征方法，包括傅里叶变换红外光谱、X射线吸收光谱（XAS）和密度泛函理论（DFT）计算，研究了CN负载的单原子催化剂中镍活性中心的局部环境。这些结果挑战了传统的结构模型，并提出了一种与当前实验证据更相符的新结构。这种新结构是迈向合理开发催化剂方法的基础步骤，有助于更精确地设计和应用这些创新型催化剂。
