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Title: Hydrothermal synthesis of highly nitrogen-doped few-layer graphene via solid–gas reaction

Highlights: • A novel approach to synthesis of N-doped few-layer graphene has been developed. • The high doping levels of N in products are achieved. • XPS and XANES results reveal a thermal transformation of N bonding configurations. • The developed method is cost-effective and eco-friendly. - Abstract: Nitrogen-doped (N-doped) graphene sheets with high doping concentration were facilely synthesized through solid–gas reaction of graphene oxide (GO) with ammonia vapor in a self-designed hydrothermal system. The morphology, surface chemistry and electronic structure of N-doped graphene sheets were investigated by TEM, AFM, XRD, XPS, XANES and Raman characterizations. Upon hydrothermal treatment, up to 13.22 at% of nitrogen could be introduced into the crumpled few-layer graphene sheets. Both XPS and XANES analysis reveal that the reaction between oxygen functional groups in GO and ammonia vapor produces amide and amine species in hydrothermally treated GO (HTGO). Subsequent thermal annealing of the resultant HTGO introduces a gradual transformation of nitrogen bonding configurations in graphene sheets from amine N to pyridinic and graphitic N with the increase of annealing temperature. This study provides a simple but cost-effective and eco-friendly method to prepare N-doped graphene materials in large-scale for potential applications.
Authors:
 [1] ;  [2] ; ; ;  [1] ; ;  [3]
  1. College of Physics Science and Technology, Guangxi University, Nanning 530004 (China)
  2. Jiangsu Key Laboratory for Carbon-Based Functional Material and Devices, Institute of Functional Nano and Soft Materials Laboratory (FUNSOM), Soochow University, Suzhou 215123 (China)
  3. Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049 (China)
Publication Date:
OSTI Identifier:
22420764
Resource Type:
Journal Article
Resource Relation:
Journal Name: Materials Research Bulletin; Journal Volume: 61; Other Information: Copyright (c) 2014 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ABSORPTION SPECTROSCOPY; AMINES; AMMONIA; ATOMIC FORCE MICROSCOPY; DOPED MATERIALS; ELECTRONIC STRUCTURE; FINE STRUCTURE; GRAPHENE; GRAPHITE; HYDROTHERMAL SYNTHESIS; HYDROTHERMAL SYSTEMS; LAYERS; MORPHOLOGY; NANOSTRUCTURES; TRANSMISSION ELECTRON MICROSCOPY; X-RAY DIFFRACTION; X-RAY PHOTOELECTRON SPECTROSCOPY; X-RAY SPECTROSCOPY