首页|N-doped 2D graphite-2H nanoplatelets (GNPs) with enhanced PMS activation performance: Structure-dependent performance and Catalytic Mechanism
N-doped 2D graphite-2H nanoplatelets (GNPs) with enhanced PMS activation performance: Structure-dependent performance and Catalytic Mechanism
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NSTL
Elsevier
The N-doped two-dimensional (2D) carbon-based catalysts play a crucial role in the PMS catalytic activity of advanced oxidation processes (AOPs). However, their activation mechanism still lacks a reasonable explanation. A low-cost and one-step synthesis of N-doped graphite-2H nanoplatelets (N-GNPs) were prepared through the calcination under 600 degrees C. N-GNPs(0.5)-600 was applied to activate permonosulfate (PMS) 19.4 times faster than that of pure PMS system under visible light to degrade bis(monochloro-s-triazine) reactive dye. We first demonstrate that electron arrangement in N-GNPs samples can effectively activate PMS and generate O-1(2) as much as SO4 center dot- and HO center dot as the main reactive species. The EPR test results were consistent with the quenching test. Density functional theory (DFT) calculations showed the graphite N adjacent C atoms (Eb= -8.9 eV) were promoted to produce more active sites. Bidirectional regulation of graphite N bonded C atoms form a local electron state, making the C most active electron donation. The 2P(z) orbital of carbon atoms becomes occupied with the free electrons. The localized orbitals lead to the stronger Columbic repulsion of pi electrons and enlarged interlayer distance, making it easier for the electrons to give out and accelerate the free-radical process. (C) 2021 Taiwan Institute of Chemical Engineers. Published by Elsevier B.V. All rights reserved.