title: Nitrogen-doped graphene for generation and evolution of reactive radicals by metal-free catalysis.
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.
authors: Department of Chemical Engineering, Curtin University , GPO Box U1987, Bentley, Western Australia 6845, Australia.
authors: Xiaoguang
authors: X
authors: Duan
authors: Zhimin
authors: Z
authors: Ao
authors: Hongqi
authors: H
authors: Sun
authors: Stacey
authors: S
authors: Indrawirawan
authors: Yuxian
authors: Y
authors: Wang
authors: Jian
authors: J
authors: Kang
authors: Fengli
authors: F
authors: Liang
authors: Z H
authors: ZH
authors: Zhu
authors: Shaobin
authors: S
authors: Wang
keywords: DFT; graphene; metal-free catalysis; nitrogen doping; peroxymonosulfate; phenol degradation