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Sulfur anchored on N-doped porous carbon as metal-free peroxymonosulfate activator for tetracycline hydrochloride degradation: Nonradical pathway mechanism, performance and biotoxicity

CHEMICAL ENGINEERING JOURNAL [2023]
Jinling Xie, Lingrui Zhang, Xuan Luo, Li Huang, Xiaobo Gong, Jing Tian
ABSTRACT

Dual heteroatoms doping is an efficient method to improve catalytic activity of carbon materials. In this research, N, S co-doped porous carbon material (S-NPC) was prepared by direct thermal reduction method of metal organic frameworks and proved to be an excellent metal-free heterogeneous Fenton-like catalyst for peroxymonosulfate (PMS) activation. Tetracycline hydrochloride (TC) could be completely degraded in a short time of 20 min with 20 mg S-NPC and 10 mg PMS at 25 °C, attributing that N, S co-doping provided more defects (I D /I G  = 0.998) to produce more active sites for PMS activation. Based on the results from radical identification, scavenging tests, density functional theory (DFT) and electrochemical analysis, non-radical pathway based on singlet oxygen ( 1 O 2 ) and electron transfer was proposed to be the dominant way in the S-NPC/PMS system and the contribution rate was about 95.872 %. Three possible pathways of TC degradation were proposed by high resolution liquid chromatography-mass spectrometry (LC-MS) and the toxicity of intermediate products was lower than TC. This study provided a novel strategy to degrade pollutants by preparing efficient co-doping metal-free Fenton-like catalyst.

MATERIALS

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