Nitrogen-doped amorphous monolayer carbon

• 成果类型: Article
• 署名作者: Bai, Xiuhui; Hu, Pengfei; Li, Ang; Zhang, Youwei; Li, Aowen; Zhang, Guangjie; Xue, Yufeng; Jiang, Tianxing; Wang, Zezhou; Cui, Hanke; Kang, Jianxin; Zhao, Hewei; Gu, Lin; Zhou, Wu; Liu, Li-Min; Qiu, Xiaohui; Guo, Lin
• 署名单位: Beihang University; Beihang University; Chinese Academy of Sciences; University of Chinese Academy of Sciences, CAS; Chinese Academy of Sciences; National Center for Nanoscience & Technology, CAS; Tsinghua University; Tsinghua University; Chinese Academy of Sciences; University of Chinese Academy of Sciences, CAS
• 刊物名称: Nature
• ISSN/ISSBN: 0028-6685
• DOI: 10.1038/s41586-024-07958-0
• 发表日期: 2024-10-03
• 页码: 80-+
• 关键词: low-temperature growth; electronic-structure; optical-properties; charge-carriers; mechanisms

摘要

Monoatomic-layered carbon materials, such as graphene(1) and amorphous monolayer carbon(2,3), have stimulated intense fundamental and applied research owing to their unprecedented physical properties and a wide range of promising applications(4,5). So far, such materials have mainly been produced by chemical vapour deposition, which typically requires stringent reaction conditions compared to solution-phase synthesis. Herein, we demonstrate the solution preparation of free-standing nitrogen-doped amorphous monolayer carbon with mixed five-, six- and seven-membered (5-6-7-membered) rings through the polymerization of pyrrole within the confined interlayer cavity of a removable layered-double-hydroxide template. Structural characterizations and first-principles calculations suggest that the nitrogen-doped amorphous monolayer carbon was formed by radical polymerization of pyrrole at the alpha, beta and N sites subjected to confinement of the reaction space, which enables bond rearrangements through the Stone-Wales transformation. The spatial confinement inhibits the C-C bond rotation and chain entanglement during polymerization, resulting in an atom-thick continuous amorphous layer with an in-plane pi-conjugation electronic structure. The spatially confined radical polymerization using solid templates and ion exchange strategy demonstrates potential as a universal synthesis approach for obtaining two-dimensional covalent networks, as exemplified by the successful synthesis of monolayers of polythiophene and polycarbazole.