Tanabe Yoichi, Ito Yoshikazu, Sugawara Katsuaki, Jeong Samuel, Ohto Tatsuhiko, Nishiuchi Tomohiko, Kawada Naoaki, Kimura Shojiro, Aleman Christopher Florencio, Takahashi Takashi, Kotani Motoko, Chen Mingwei
Department of Applied Science, Okayama University of Science, Okayama, 700-0005, Japan.
Institute of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba, Ibaraki, 305-8573, Japan.
Adv Mater. 2022 Dec;34(51):e2205986. doi: 10.1002/adma.202205986. Epub 2022 Nov 18.
Nitrogen (N) doping is one of the most effective approaches to tailor the chemical and physical properties of graphene. By the interplay between N dopants and 3D curvature of graphene lattices, N-doped 3D graphene displays superior performance in electrocatalysis and solar-energy harvesting for energy and environmental applications. However, the electrical transport properties and the electronic states, which are the key factors to understand the origins of the N-doping effect in 3D graphene, are still missing. The electronic properties of N-doped 3D graphene are systematically investigated by an electric-double-layer transistor method. It is demonstrated that Urbach-tail-like localized states are located around the neutral point of N-doped 3D graphene with the background metallic transport channels. The dual nature of electronic states, generated by the synergistic effect of N dopants and 3D curvature of graphene, can be the electronic origin of the high electrocatalysis, enhanced molecular adsorption, and light absorption of N-doped 3D graphene.
氮（N）掺杂是调整石墨烯化学和物理性质最有效的方法之一。通过氮掺杂剂与石墨烯晶格三维曲率之间的相互作用，氮掺杂三维石墨烯在用于能源和环境应用的电催化及太阳能收集方面表现出卓越性能。然而，作为理解三维石墨烯中氮掺杂效应起源的关键因素，其电输运性质和电子态仍不清楚。采用双层电晶体管方法对氮掺杂三维石墨烯的电子性质进行了系统研究。结果表明，在具有背景金属传输通道的氮掺杂三维石墨烯中性点周围存在类乌尔巴赫尾局域态。由氮掺杂剂与石墨烯三维曲率的协同效应产生的电子态的双重性质，可能是氮掺杂三维石墨烯高电催化性、增强分子吸附及光吸收的电子起源。
