Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis
|dc.identifier.citation||Duan, X. and Ao, Z. and Sun, H. and Indrawirawan, S. and Wang, Y. and Kang, J. and Liang, F. et al. 2015. Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis. ACS Applied Materials and Interfaces. 7 (7): pp. 4169-4178.|
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 Ndoped 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 Ndopedgraphene. 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.
|dc.publisher||American Chemical Society|
|dc.title||Nitrogen-Doped Graphene for Generation and Evolution of Reactive Radicals by Metal-Free Catalysis|
|dcterms.source.title||ACS Applied Materials and Interfaces|
|curtin.department||Department of Chemical Engineering|
|curtin.accessStatus||Fulltext not available|