Synthesis of metal-free nitrogen-doped mesoporous carbon nanosheets with reference to molecular self-assembly for efficient peroxymonosulfate activation

The application of metal-free carbon materials in Sulfate radical-based advanced oxidation processes (SR-AOPs) has attracted great attention. In SR-AOPs, porosity and active sites are the keys for nitrogen-doped carbon materials to exhibit high catalytic activity. In this paper, melamine and gallic acid were selected as raw materials, preparing metal-free nitrogen-doped carbon materials by using the molecular self-assembly synthesis method. The catalysts with different structural morphology and surface chemistry were obtained by controlling the pyrolysis temperature. It proposed the formation mechanism of nitrogen-doped mesoporous carbon nanosheets (NMC). The pyrolysis temperature was critical for the regulation of surface properties as well as the structure of carbon materials. It was found that NMC-800 exhibited fluffy and porous microstructure, and various active sites on the surface of the catalyst, including graphite N, pyridine N and C O. In the NMC-800/PMS system, the SMX degradation efficiency and corresponding rate constant could achieve 90.3 % and 0.1705 min −1 , respectively. Besides, the degradation pathways and intermediate products of SMX were discussed by the analysis of quenching experiments, electron spin resonance (ESR) and liquid chromatography-mass spectrometry (LC-MS). • Metal-free nitrogen-doped carbon materials were prepared by reference to molecular self-assembly. • NMC-800 exhibited excellent PMS activation properties. • Non-radical singlet oxygen was the main reactive oxygen species. • Pyridine N, graphite N and C O were the main active sites.