Synthesis of N-doped graphene film with tunable graphitic and pyridinic doping content

Nitrogen-doped (N-doped) graphene films with up to a 17.39 at.% doping level were synthesized with the chemical vapor deposition growth method. An extensive range of tunable nitrogen doping levels was achieved by selecting organic molecules as precursors grown at a wide temperature range of 300 to 1000 °C. The benzene rings in the precursor significantly reduced the energy requirements of N-doped graphene. The incorporation of bridgehead nitrogen and amino groups ensured a high nitrogen doping level and offered the tunable modulation of nitrogen dopant concentrations. The influence of temperature on the nitrogen content was investigated, distinguishing the graphitic and pyridinic dopant types, each demonstrating unique trends considering the dopant stability and growth mechanism. Specifically, the proportion of graphitic doping could be modulated from 40 % to 100 %. Notably, the pyrrolic type was absent at lower temperatures and was nearly negligible at elevated temperatures. Therefore, we developed a synthesis method for N-doped graphene growth that allowed for the selective and prioritized tuning of nitrogen dopant types. This method is particularly favorable when specific nitrogen dopants at certain doping levels are required for electrical and chemical catalytic applications.