Space‐Confined Synthesis of Monolayer Graphdiyne in MXene Interlayer

Abstract

Graphdiyne (GDY) is an artificial carbon allotrope that is conceptually similar to graphene but composed of sp‐ and sp2‐hybridized carbon atoms. Monolayer GDY (ML‐GDY) is predicted to be an ideal two‐dimensional (2D) semiconductor material with a wide range of applications. However, its synthesis has posed a significant challenge, leading to difficulties in experimentally validating theoretical properties. Here, we report that in‐situ acetylenic homocoupling of hexaethynylbenzene within the sub‐nanometer interlayer space of MXene can effectively prevent out‐of‐plane growth or vertical stacking of the material, resulting in ML‐GDY with in‐plane periodicity. The subsequent exfoliation process successfully yields free‐standing GDY monolayers with micrometer‐scale lateral dimensions. The fabrication of field‐effect transistor on free‐standing ML‐GDY makes the first measurement of its electronic properties possible. The measured electrical conductivity (5.1×103 S m−1) and carrier mobility (231.4 cm2 V−1 s−1) at room temperature are remarkably higher than those of the previously reported multilayer GDY materials. The space‐confined synthesis using layered crystals as templates provides a new strategy for preparing 2D materials with precisely controlled layer numbers and long‐range structural order.This article is protected by copyright. All rights reserved

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“…(i) I ds – V ds features of ML-GDY measured at 298 K. The top-left inset is a top-view SEM image of the device, and the bottom-right inset is a cross-sectional HAADF-STEM image of the device. Reproduced with permission from ref . Copyright 2023 Wiley-VCH.…”

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