Mendieta-Moreno Jesús I, Mallada Benjamin, de la Torre Bruno, Cadart Timothée, Kotora Martin, Jelínek Pavel
Institute of Physics of Czech Academy of Sciences, 16200, Prague, Czech Republic.
Regional Centre of Advanced Technologies and Materials, Czech Advanced Technology and Research Institute (CATRIN), Palacký University Olomouc, 78371, Olomouc, Czech Republic.
Angew Chem Int Ed Engl. 2022 Dec 12;61(50):e202208010. doi: 10.1002/anie.202208010. Epub 2022 Nov 15.
Chemical transformation of polyaromatic hydrocarbon (PAH) molecules following different reaction strategies has always been the focus of organic synthesis. In this work, we report the synthesis of a PAH molecule, formation of which consists of an unusual C-C bond cleavage accompanied by a complex π-conjugated molecular scaffold rearrangement. We demonstrate that the complex chemical transformation is steered by concerted motion of individual Au gold atoms on a supporting Au(111) surface. This observation underpins the importance of single-atom catalysis mediated by adatoms in on-surface synthesis as well as catalytic activity of single Au atoms facilitating cleavage of covalent carbon bonds.
遵循不同反应策略的多环芳烃（PAH）分子的化学转化一直是有机合成的重点。在这项工作中，我们报告了一种PAH分子的合成，其形成过程包括不寻常的C-C键断裂以及复杂的π共轭分子骨架重排。我们证明，这种复杂的化学转化是由单个金原子在支撑的Au(111)表面上的协同运动所引导的。这一观察结果强调了表面合成中由吸附原子介导的单原子催化的重要性，以及单个金原子促进共价碳碳键断裂的催化活性。
