Dense arrangement of crown ethers in graphene: novel graphitic carbon oxides with enhanced optoelectronic properties

Abstract

Incorporating crown ethers into a graphene lattice presents an efficient means of tuning its properties and expanding its range of potential applications. This study employed density functional theory calculations to introduce a series of novel graphitic carbon oxides through the dense arrangement of crown ethers featuring varying cavity sizes within the graphene structure. These newly developed graphitic carbon oxides exhibit thermodynamic and dynamic stability. They also manifest improved stability relative to previously reported graphene oxides with similar oxygen content. Notably, a robust linear relationship is observed between the cohesive energies and the proportion of oxygen atoms. The electronic properties of these graphitic carbon oxides span a spectrum of characteristics, including semi-metallic, metallic, and semi-conducting behavior. Their calculated band gaps range from 0.11 eV to 4.38 eV. Specifically, our analysis reveals that C6G-1, characterized by its largest crown ether-like nanopore with six oxygen atoms, holds potential as a material for photocatalytic water splitting. Moreover, these materials exhibit anisotropic optical properties, showcasing a significant enhancement in absorption within the infrared and visible regions relative to pristine graphene. Given the successful experimental synthesis of crown ether in graphene, we anticipate that our findings will contribute to the widespread utilization of graphene derivatives in low-dimensional electronic, catalytic, and optical devices.