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Cu/N co-doped biochar activating PMS for selective degrading paracetamol via a non-radical pathway dominated by singlet oxygen and electron transfer

Journal 2024 · IF 8.1 · 发表于 2024 年 4 月 17 日
作者: Que Wu,Yongqing Zhang,Hong Meng,Xuefeng Wu,Yuqi Liu,Li Li
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摘要

The non-free radical oxidation pathway (PMS-NOPs) of peroxymonosulfate (PMS) holds significant promise for practical wastewater treatment applications, owing to its low oxidation potential, high PMS utilization rate, and robust anti-interference capability in the degradation of pollutants. A novel activator copper nitrogen co-doped porous biochar (Cu-N-BC) with rich defect edges and functional groups was obtained by adding Cu and N to the biochar matrix generated by sodium alginate through pyrolysis in this study. Under the condition of 1 mM PMS, 30 mg/L activator was used to activate PMS and achieve efficient degradation of 10 mg/L paracetamol (PCT) within 15 min, with a high reaction rate constants (k obs ) of 0.391 min −1 . The activation mechanism of the Cu-N-BC/PMS/PCT system was a non-radical activation pathway with the dominance of singlet oxygen ( 1 O 2 ) and the presence of catalyst-mediated electron transfer. The graphite nitrogen, pyridine nitrogen, and Cu–N coordination introduced by Cu/N co-doping, as well as the carbon skeleton and C O functional group of biochar, were considered active sites that promote the 1 O 2 generation. The Cu-N-BC/PMS system exhibits strong stability, eco-friendliness, effective mineralization, and interference resistance across diverse pH levels (3–11) and interfering ions, including Cl − , H 2 PO 4 − , NO 3 − , SO 4 2− , and humic acid. Remarkably, it efficiently degrades PCT in tap and lake water, achieving a notable 63.73% TOC mineralization rate, with leached copper ions below 0.02 mg/L. This research introduces a novel method for obtaining metal nitrogen carbon activators and enhances understanding of PMS non-radical activation pathways and active sites.