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|Title:||Nitrogen-doped graphene for generation and evolution of reactive radicals by metal-free catalysis|
|Citation:||ACS Applied Materials and Interfaces, 2015; 7(7):4169-4178|
|Publisher:||American Chemical Society|
|Xiaoguang Duan, Zhimin Ao, Hongqi Sun, Stacey Indrawirawan, Yuxian Wang, Jian Kang, Fengli Liang, Z.H. Zhu, and Shaobin Wang|
|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:||Nitrogen doping; graphene; peroxymonosulfate; phenol degradation; metal-free catalysis; DFT|
|Description:||Published: January 29, 2015|
|Rights:||© 2015 American Chemical Society|
|Appears in Collections:||Chemical Engineering publications|
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