Abstract
The ability to change the secondary electron emission properties of nitrogen-doped graphene (N-graphene) has been demonstrated. To this end, a novel microwave plasma-enabled scalable route for continuous and controllable fabrication of free-standing N-graphene sheets was developed. High-quality N-graphene with prescribed structural qualities was produced at a rate of 0.5 mg/min by tailoring the high energy density plasma environment. Up to 8% of nitrogen doping levels were achieved while keeping the oxygen content at residual amounts (~ 1%). The synthesis is accomplished via a single step, at atmospheric conditions, using ethanol/methane and ammonia/methylamine as carbon and nitrogen precursors. The type and level of doping is affected by the position where the N-precursor is injected in the plasma environment and by the type of precursors used. Importantly, N atoms incorporated predominantly in pyridinic/pyrrolic functional groups alter the performance of the collective electronic oscillations, i.e. plasmons, of graphene. For the first time it has been demonstrated that the synergistic effect between the electronic structure changes and the reduction of graphene π-plasmons caused by N doping, along with the peculiar “crumpled” morphology, leads to sub-unitary (< 1) secondary electron yields. N-graphene can be considered as a prospective low secondary electron emission and plasmonic material.
Highlights
The ability to change the secondary electron emission properties of nitrogen-doped graphene (N-graphene) has been demonstrated
The visible curling at the edges of the sheets seen in the high resolution transmission electron microscopy (HRTEM) images allows for an estimation of their thickness
This work shows that N-graphene, in particular N-graphene with predominant pyridinic/pyrrolic bonding configurations, can be exploited to reduce the Secondary Electron Emission (SEE) of carbon materials
Summary
The ability to change the secondary electron emission properties of nitrogen-doped graphene (N-graphene) has been demonstrated. The end-result is production of graphene sheets, highly doped by nitrogen (up to 8%at.), collected with ~ 40% in the form of single atomic layers, with very low-content of oxygen (< 1%) and high-ratio of sp2/sp[3] carbons (~ 15)[24,25,26,27,28,29,30,31]. It provides the ability to control the amount and localization of energy and matter delivered from plasma bulk to developing nanostructures at atomic scale level, the key to achieve the desired morphological, electronic and functional properties of targeted materials.
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