Qin Tianchen, Liang Baiyao, Hu Lei, Xu Qian, Wang Tao, Zhu Junfa
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China.
State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, Shanghai, 200032, China.
Chemphyschem. 2025 Jan 14;26(2):e202400601. doi: 10.1002/cphc.202400601. Epub 2024 Nov 11.
The recent developed bottom-up on-surface synthesis offers unprecedent opportunities for the fabrication of two-dimensional (2D) carbon-based networks with atomic precision. Hierarchical coupling approach has been proposed as an efficient strategy for improving the corresponding reaction selectivity and quality of target structures. Herein, we report the synthesis of a nitrogen-doped carbon-based network on Ag(100) utilizing a hierarchical Ullmann coupling strategy. The accurate identification of reaction intermediates and products by scanning tunneling microscopy allows us to unravel the reaction mechanism. The synthetic process of 2D carbon-based networks is kinetics-driven, relying on the competition between dechlorination and C-C coupling. We expect that our discussion on the mechanism of hierarchical coupling may shed light on the rational design and precise synthesis of 2D carbon-based networks on surfaces.
最近发展起来的自下而上的表面合成方法为精确制备具有原子精度的二维（2D）碳基网络提供了前所未有的机会。分层耦合方法已被提出作为提高相应反应选择性和目标结构质量的有效策略。在此，我们报道了利用分层乌尔曼耦合策略在Ag(100)上合成氮掺杂碳基网络。通过扫描隧道显微镜对反应中间体和产物的精确识别使我们能够揭示反应机理。二维碳基网络的合成过程是由动力学驱动的，依赖于脱氯和C-C耦合之间的竞争。我们期望我们对分层耦合机理的讨论能够为表面二维碳基网络的合理设计和精确合成提供启示。
