Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis
Top Cited Papers
- 9 February 2015
- journal article
- research article
- Published by American Chemical Society (ACS) in ACS Applied Materials & Interfaces
- Vol. 7 (7), 4169-4178
- https://doi.org/10.1021/am508416n
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.Keywords
Funding Information
- Australian Research Council (DP130101319)
- Curtin University of Technology
This publication has 49 references indexed in Scilit:
- N-Doping-Induced Nonradical Reaction on Single-Walled Carbon Nanotubes for Catalytic Phenol OxidationACS Catalysis, 2014
- Nanocarbons for the Development of Advanced CatalystsChemical Reviews, 2013
- Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reactionEnergy & Environmental Science, 2012
- Nitrogen‐Doped Carbon Nanotubes as a Highly Active Metal‐Free Catalyst for Selective OxidationChemSusChem, 2011
- Graphene and Graphene Oxide: Synthesis, Properties, and ApplicationsAdvanced Materials, 2010
- Metal‐Free Heterogeneous Catalysis for Sustainable ChemistryChemSusChem, 2010
- The chemistry of grapheneJournal of Materials Chemistry, 2010
- The rise of grapheneNature Materials, 2007
- Cobalt-Mediated Activation of Peroxymonosulfate and Sulfate Radical Attack on Phenolic Compounds. Implications of Chloride IonsEnvironmental Science & Technology, 2005
- Degradation of Organic Contaminants in Water with Sulfate Radicals Generated by the Conjunction of Peroxymonosulfate with CobaltEnvironmental Science & Technology, 2003