Ye Bo-Chao, Li Wen-Hao, Zhang Xia, Chen Jian, Gao Yong, Wang Dingsheng, Pan Hongge
Department of Chemistry, Tsinghua University, Beijing, 100084, China.
Department of Chemistry, Northeastern University, Shenyang, 110819, China.
Adv Mater. 2024 Nov;36(45):e2402747. doi: 10.1002/adma.202402747. Epub 2024 Sep 18.
For traditional metal complexes, intricate chemistry is required to acquire appropriate ligands for controlling the electron and steric hindrance of metal active centers. Comparatively, the preparation of single-atom catalysts is much easier with more straightforward and effective accesses for the arrangement and control of metal active centers. The presence of coordination atoms or neighboring functional atoms on the supports' surface ensures the stability of metal single-atoms and their interactions with individual metal atoms substantially regulate the performance of metal active centers. Therefore, the collaborative interaction between metal and the surrounding coordination environment enhances the initiation of reaction substrates and the formation and transformation of crucial intermediate compounds, which imparts single-atom catalysts with significant catalytic efficacy, rendering them a valuable framework for investigating the correlation between structure and activity, as well as the reaction mechanism of catalysts in organic reactions. Herein, comprehensive overviews of the coordination interaction for both homogeneous metal complexes and single-atom catalysts in organic reactions are provided. Additionally, reflective conjectures about the advancement of single-atom catalysts in organic synthesis are also proposed to present as a reference for later development.
对于传统金属配合物而言,需要复杂的化学过程来获得合适的配体,以控制金属活性中心的电子和空间位阻。相比之下,单原子催化剂的制备要容易得多,能够以更直接有效的方式来排列和控制金属活性中心。载体表面配位原子或相邻功能原子的存在确保了金属单原子的稳定性,并且它们与单个金属原子的相互作用极大地调节了金属活性中心的性能。因此,金属与周围配位环境之间的协同相互作用增强了反应底物的引发以及关键中间化合物的形成和转化,这赋予了单原子催化剂显著的催化效能,使其成为研究结构与活性之间的相关性以及有机反应中催化剂反应机理的有价值框架。在此,本文对均相金属配合物和单原子催化剂在有机反应中的配位相互作用进行了全面综述。此外,还对单原子催化剂在有机合成中的进展提出了反思性猜想,以供后续发展参考。