Maddi Chiranjeevi, Bourquard Florent, Barnier Vincent, Avila José, Asensio Maria-Carmen, Tite Teddy, Donnet Christophe, Garrelie Florence
Univ Lyon, Université Jean Monnet, Laboratoire Hubert Curien UMR 5516, F- 42000, Saint-Étienne, France.
Laboratoire Georges Friedel, Ecole Nationale Supérieure des Mines, F-42023, Saint-Etienne, France.
Sci Rep. 2018 Feb 19;8(1):3247. doi: 10.1038/s41598-018-21639-9.
New synthesis routes to tailor graphene properties by controlling the concentration and chemical configuration of dopants show great promise. Herein we report the direct reproducible synthesis of 2-3% nitrogen-doped 'few-layer' graphene from a solid state nitrogen carbide a-C:N source synthesized by femtosecond pulsed laser ablation. Analytical investigations, including synchrotron facilities, made it possible to identify the configuration and chemistry of the nitrogen-doped graphene films. Auger mapping successfully quantified the 2D distribution of the number of graphene layers over the surface, and hence offers a new original way to probe the architecture of graphene sheets. The films mainly consist in a Bernal ABA stacking three-layer architecture, with a layer number distribution ranging from 2 to 6. Nitrogen doping affects the charge carrier distribution but has no significant effects on the number of lattice defects or disorders, compared to undoped graphene synthetized in similar conditions. Pyridinic, quaternary and pyrrolic nitrogen are the dominant chemical configurations, pyridinic N being preponderant at the scale of the film architecture. This work opens highly promising perspectives for the development of self-organized nitrogen-doped graphene materials, as synthetized from solid carbon nitride, with various functionalities, and for the characterization of 2D materials using a significant new methodology.
通过控制掺杂剂的浓度和化学构型来定制石墨烯特性的新合成路线显示出巨大的潜力。在此，我们报告了从飞秒脉冲激光烧蚀合成的固态氮化物a-C:N源直接可重复合成2-3%氮掺杂的“少层”石墨烯。包括同步加速器设施在内的分析研究使得确定氮掺杂石墨烯薄膜的构型和化学性质成为可能。俄歇映射成功地量化了表面上石墨烯层数的二维分布，因此提供了一种探测石墨烯片层结构的全新方法。这些薄膜主要由伯纳尔ABA堆叠的三层结构组成，层数分布范围为2至6。与在类似条件下合成的未掺杂石墨烯相比，氮掺杂影响电荷载流子分布，但对晶格缺陷或无序数量没有显著影响。吡啶型、季铵型和吡咯型氮是主要的化学构型，在薄膜结构尺度上吡啶型N占主导。这项工作为开发由固体碳氮化物合成的具有各种功能的自组织氮掺杂石墨烯材料，以及使用一种重要的新方法对二维材料进行表征开辟了极有前景的前景。
