Toward N-Doped Graphene via Solvothermal Synthesis

TLDR

Theoretical studies predict that nitrogen doping can tailor graphene’s electronic properties, but experimental work is limited by a lack of scalable synthesis methods. The authors aim to develop a scalable, one‑pot synthesis of N‑doped graphene using tetrachloromethane and lithium nitride. The method involves reacting tetrachloromethane with lithium nitride under mild conditions to produce gram‑scale N‑doped graphene. Scanning tunnelling microscopy reveals nitrogen‑induced electronic perturbations, with nitrogen content ranging from 4.5 % to 16.4 %, and the resulting N‑doped graphene shows superior catalytic activity in fuel‑cell cathode oxygen‑reduction reactions compared to pure graphene and commercial carbon black, indicating expanded application potential.

Abstract

Theoretical studies predicted that doping graphene with nitrogen can tailor its electronic properties and chemical reactivity. However, experimental investigations are still limited because of the lack of synthesis techniques that can deliver a reasonable quantity. We develop here a novel method for one-pot direct synthesis of N-doped graphene via the reaction of tetrachloromethane with lithium nitride under mild conditions, which renders fabrication in gram scale. The distinct electronic structure perturbation induced by the incorporation of nitrogen in the graphene network is observed for the first time by scanning tunnelling microscopy. The nitrogen content varies in the range of 4.5−16.4%, which allows further modulation of the properties. The enhanced catalytic activity is demonstrated in a fuel cell cathode oxygen reduction reaction with respect to pure graphene and commercial carbon black XC-72. The resulting N-doped materials are expected to broaden the already widely explored potential applications for graphene.