Nitrogen-Nitrogen Bonds Violate Stability of N-Doped Graphene

TL;DR

This study investigates the stability of nitrogen-doped graphene, revealing that N-N bonds compromise stability and providing insights into optimal nitrogen incorporation for stable structures at high temperatures.

Contribution

It introduces a combined computational approach to determine stable nitrogen doping levels in graphene and highlights the destabilizing effect of N-N bonds.

Findings

N-N bonds reduce stability of N-doped graphene

Stable N-doped structures can contain up to 28 nitrogen atoms

Electron density distribution varies with structural pattern

Abstract

Two-dimensional alloys of carbon and nitrogen represent an urgent interest due to prospective applications in nanomechanical and optoelectronic devices. Stability of these chemical structures must be understood as a function of their composition. The present study employs hybrid density functional theory and reactive molecular dynamics simulations to get insights regarding how many nitrogen atoms can be incorporated into the graphene sheet without destroying it. We conclude that (1) C:N=56:28 structure and all nitrogen-poorer structures maintain stability at 1000 K; (2) stability suffers from N-N bonds; (3) distribution of electron density heavily depends on the structural pattern in the N-doped graphene. Our calculations support experimental efforts on the production of highly N-doped graphene and tuning mechanical and optoelectronic properties of graphene.