Deposition of N-doped graphene and its mechanism study via in situ mass spectrometry†

Abstract

Nitrogen doping of graphene is one of the most effective methods to open the zero-band gap of graphene, presenting a promising approach to modify its electronic structure. In this report, we introduce a novel method for growing large-area N-doped graphene directly on copper foil using atmospheric-pressure chemical vapor deposition (APCVD) using the pyrolysis of acetonitrile. In situ mass spectrometry combined with APCVD gave insights into the contribution and behavior of different species during the formation of N-doped graphene. Density functional theory calculations, paired with experimental results, were employed to study the growth mechanism of N-doped graphene with acetonitrile. Furthermore, the synthesized N-doped graphene was investigated as an electrode material for vanadium redox flow batteries (VRFB), focusing on its catalytic activity for the V(IV)/V(V) redox reaction. These findings not only deepen our understanding of the growth mechanisms of N-doped graphene but also provide a foundation for its application in energy storage systems, offering guidance for the synthesis of doped graphene and carbon nanotubes for advanced electrode materials in VRFB and beyond.