Liu Hua-Wei, He Peng, Li Wen-Tao, Sun Wei, Shi Kai, Wang You-Qin, Mo Qian-Kun, Zhang Xin-Yu, Zhu Shou-Fei
Frontiers Science Center for New Organic Matters, State Key Laboratory and Institute of Elemento-Organic Chemistry, College of Chemistry, Nankai University, 94th Weijin Road, Tianjin, 300071, China.
Angew Chem Int Ed Engl. 2023 Oct 26;62(44):e202309111. doi: 10.1002/anie.202309111. Epub 2023 Sep 25.
Recently, the application of computational tools to the rational design of catalysts has received considerable attention, but progress has been limited by the reliance on databases and because mechanistic data have been almost neglected. Herein, we report a new strategy for catalyst design, designated catalyst-oriented design based on elementary reactions (CODER), which fully utilizes mechanistic data, combines the strengths of computational tools and researcher experience. CODER enabled the development of extremely efficient Pd catalysts for C-N coupling, which markedly improved the efficiency of the synthesis of widely used triarylamine optoelectronic materials by enhancing the turnover numbers (up to 340000) to 1-3 orders of magnitude towards literature values.
最近，计算工具在催化剂合理设计中的应用受到了广泛关注，但由于对数据库的依赖以及几乎忽略了机理数据，进展有限。在此，我们报告了一种新的催化剂设计策略，即基于基元反应的面向催化剂设计（CODER），该策略充分利用机理数据，结合了计算工具和研究人员经验的优势。CODER使得开发出用于C-N偶联的极其高效的钯催化剂成为可能，通过将周转数（高达340000）提高到比文献值高1 - 3个数量级，显著提高了广泛使用的三芳基胺光电材料的合成效率。
