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Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis

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Department of Chemical Engineering, Curtin University, GPO Box U1987, Bentley, Western Australia 6845, Australia
Centre for Clean Energy Technology, School of Chemistry and Forensic Science, University of Technology, Sydney, PO Box 123, Sydney, New South Wales 2007, Australia
§ School of Chemical Engineering, The University of Queensland, St Lucia, Queensland 4072, Australia
*S. Wang. E-mail: [email protected]. Phone: +61 8 9266 3776.
*H. Sun. E-mail: [email protected]. Phone: +61 8 9266 9211.
Cite this: ACS Appl. Mater. Interfaces 2015, 7, 7, 4169–4178
Publication Date (Web):January 29, 2015
https://doi.org/10.1021/am508416n
Copyright © 2015 American Chemical Society
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Abstract

N-Doped graphene (NG) nanomaterials were synthesized by directly annealing graphene oxide (GO) with a novel nitrogen precursor of melamine. A high N-doping level, 8–11 at. %, was achieved at a moderate temperature. The sample of NG-700, obtained at a calcination temperature of 700 °C, showed the highest efficiency in degradation of phenol solutions by metal-free catalytic activation of peroxymonosulfate (PMS). The catalytic activity of the N-doped rGO (NG-700) was about 80 times higher than that of undoped rGO in phenol degradation. Moreover, the activity of NG-700 was 18.5 times higher than that of the most popular metal-based catalyst of nanocrystalline Co3O4 in PMS activation. Theoretical calculations using spin–unrestricted density functional theory (DFT) were carried out to probe the active sites for PMS activation on N-doped graphene. In addition, experimental detection of generated radicals using electron paramagnetic resonance (EPR) and competitive radical reactions was performed to reveal the PMS activation processes and pathways of phenol degradation on nanocarbons. It was observed that both OH and SO4•– existed in the oxidation processes and played critical roles for phenol oxidation.

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Preparation procedures of GO, N-rGO-350, N-CNT-350, and nanocrystalline Co3O4; FTIR, TGA, XPS C 1s spectra; test of intermediates, TOC, kinetic studies, and EPR spectra. The material is available free of charge via the Internet at http://pubs.acs.org.

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