Nitrogen-doped amorphous monolayer carbon

Xiuhui Bai, Pengfei Hu, Ang Li, Youwei Zhang, Aowen Li, Guangjie Zhang, Yufeng Xue, Tianxing Jiang, Zezhou Wang, Hanke Cui, Jianxin Kang, Hewei Zhao, Lin Gu (), Wu Zhou (), Li-Min Liu (), Xiaohui Qiu () and Lin Guo ()
Additional contact information
Xiuhui Bai: Beihang University
Pengfei Hu: Beihang University
Ang Li: University of Chinese Academy of Sciences
Youwei Zhang: Beihang University
Aowen Li: University of Chinese Academy of Sciences
Guangjie Zhang: National Center for Nanoscience and Technology
Yufeng Xue: Beihang University
Tianxing Jiang: Beihang University
Zezhou Wang: Beihang University
Hanke Cui: Beihang University
Jianxin Kang: Beihang University
Hewei Zhao: Beihang University
Lin Gu: Tsinghua University
Wu Zhou: University of Chinese Academy of Sciences
Li-Min Liu: Beihang University
Xiaohui Qiu: National Center for Nanoscience and Technology
Lin Guo: Beihang University

Nature, 2024, vol. 634, issue 8032, 80-84

Abstract: Abstract Monoatomic-layered carbon materials, such as graphene1 and amorphous monolayer carbon2,3, have stimulated intense fundamental and applied research owing to their unprecedented physical properties and a wide range of promising applications4,5. 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 α, β 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 π-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.

Date: 2024
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DOI: 10.1038/s41586-024-07958-0

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