Nitrogen-doped graphene for generation and evolution of reactive radicals by metal-free catalysis

Duan, Xiaoguang, Ao, Zhimin, Sun, Hongqi, Indrawirawan, Stacey, Wang, Yuxian, Kang, Jian, Liang, Fengli, Zhu, Zhong Hua and Wang, Shaobin (2015) Nitrogen-doped graphene for generation and evolution of reactive radicals by metal-free catalysis. ACS Applied Materials and Interfaces, 7 7: 4169-4178. doi:10.1021/am508416n


Author Duan, Xiaoguang
Ao, Zhimin
Sun, Hongqi
Indrawirawan, Stacey
Wang, Yuxian
Kang, Jian
Liang, Fengli
Zhu, Zhong Hua
Wang, Shaobin
Title Nitrogen-doped graphene for generation and evolution of reactive radicals by metal-free catalysis
Journal name ACS Applied Materials and Interfaces   Check publisher's open access policy
ISSN 1944-8252
1944-8244
Publication date 2015-01-29
Year available 2015
Sub-type Article (original research)
DOI 10.1021/am508416n
Open Access Status DOI
Volume 7
Issue 7
Start page 4169
End page 4178
Total pages 10
Place of publication Washington, United States
Publisher American Chemical Society
Language eng
Formatted 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.
Keyword DFT
graphene
metal-free catalysis
nitrogen doping
peroxymonosulfate
phenol degradation
Q-Index Code C1
Q-Index Status Confirmed Code
Institutional Status UQ

Document type: Journal Article
Sub-type: Article (original research)
Collections: School of Chemical Engineering Publications
Official 2016 Collection
 
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