期刊
CHEMOSPHERE
卷 191, 期 -, 页码 389-399出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.chemosphere.2017.10.076
关键词
Metal-free catalysis; N-rGO aerogel; Advanced oxidation; Activation mechanism; Adsorption modeling
资金
- Startup Funding of Distinguished Professorship of 1000 Talents Program [31370086963030]
- Taishan Scholar Program [11370085961006]
- Shandong Provincial Science and Technology Major Project [2015ZDZX11008, 2015GGE27286, 2016GGX104001]
- Fundamental Research Funds of Shandong University at Shandong University [2016JC005]
- Fundamental Research Funds of Shandong University [2015JC033]
3D porous N-doped reduced graphene oxide (N-rGO) aerogels were synthesized by a hydrothermal reduction of graphene oxide (GO) with urea and following freeze-drying process. N-rGO aerogels have a high BET surface of 499.70 m(2)/g and a high N doping content (5.93-7.46 at%) including three kinds of N (graphitic, pyridinic and pyrrolic). Their high catalytic performance for phenol oxidation in aqueous solution was investigated by catalytic activation of persulfate (PS). We have demonstrated that N-rGO aerogels are promising metal-free catalysts for phenol removal. Kinetics studies indicate that phenol degradation follows first-order reaction kinetics with the reaction rate constant of 0.16799 min(-1) for NrGO-A(1:30). Interestingly, the comparison of direct catalytic oxidation with adsorption-catalytic oxidation experiments indicates that adsorption plays an important role in the catalytic oxidation of phenol by decreasing the phenol degradation time. Spin density and adsorption modeling demonstrates that graphitic N in N-rGO plays the most important role for the catalytic performance by inducing high positive charge densities to adjacent carbon atoms and facilitating phenol adsorption on these carbon sites. Furthermore, the activation mechanism of persulfate (PS) on N-rGO was first investigated by DFT method and PS can be activated to generate strongly oxidative radical (SO4.(-)) by transferring electrons to N-rGO. (C) 2017 Elsevier Ltd. All rights reserved.
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