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Synthesis of monolayer and persistent bilayer graphene fragments by using a radical-mediated coupling approach
Nature Synthesis Pub Date : 2023-06-15 , DOI: 10.1038/s44160-023-00348-w
Tianyu Jiao , Yong Ni , Tingting Xu , Xudong Hou , Shaofei Wu , Longbin Ren , Yanwei Gu , Xiaohe Miao , Zhe Sun , Jishan Wu

Atomically precise single-layer graphene fragments show size- and edge-dependent electronic properties and are promising materials for electronics, photonics and spintronics. However, their synthesis has been limited to a few types of reactions. In addition, bilayer graphene fragments can exhibit intriguing properties originating from interlayer electronic interactions, but attaining a stable bilayer structure remains challenging. Here we report a synthetic strategy to prepare large-size single-layer graphene fragments by using intramolecular radical-mediated coupling reactions. One of the obtained open-shell graphene fragments demonstrates a closely stacked bilayer structure in solid state via strong intermolecular radical–radical interaction, which can be classified as delocalized ‘32-centre-2-electron’ pancake bonding. The bilayer structure is persistent in solution and dissociates only at highly oxidized states. The electronic properties of the graphene fragments were investigated. This study provides an intramolecular/intermolecular radical-mediated/radical–radical coupling approach towards diverse single-layer, bilayer and possibly multilayer graphene fragments with tunable properties.



中文翻译:

使用自由基介导的偶联方法合成单层和持久双层石墨烯片段

原子级精确的单层石墨烯片段显示出尺寸和边缘相关的电子特性,是电子、光子学和自旋电子学领域有前途的材料。然而,它们的合成仅限于几种类型的反应。此外,双层石墨烯片段可以表现出源自层间电子相互作用的有趣特性,但获得稳定的双层结构仍然具有挑战性。在这里,我们报告了一种利用分子内自由基介导的偶联反应制备大尺寸单层石墨烯片段的合成策略。所获得的开壳石墨烯片段之一通过强烈的分子间自由基-自由基相互作用表现出固态的紧密堆叠的双层结构,这可以归类为离域的“32-中心-2-电子”薄饼键合。双层结构在溶液中持久存在,并且仅在高度氧化状态下解离。研究了石墨烯碎片的电子特性。这项研究提供了一种分子内/分子间自由基介导/自由基-自由基耦合方法,用于具有可调特性的各种单层、双层和可能的多层石墨烯片段。

更新日期:2023-06-19
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