The application of heterogeneous metal-free catalysis for non-radical peroxymonosulfate (PMS) oxidation is of great significance because of its low environmental effects and mild oxidant dosage. The purpose of this study was to investigate the activation mechanism of PMS using acid-modified activated carbon and oxytetracycline (OTC) as a representative pollutant. Modified activated carbon (MAC)/PMS system was capable of achieving 100 % degradation efficiency of OTC within 60 min, with an observed rate constant () of 0.0414 min. The degradation of OTC is dominated by non-radical oxidation pathways involved in mediated singlet oxygen (O) and electron-transfer process through electron paramagnetic resonance (EPR) and radicals quenching studies. The activation of PMS is attributed to the structural defects of MAC, persistent free radicals, and oxygen functional groups such as C-OOH. Moreover, the MAC/PMS system consistently demonstrates high and reliable contaminant removal in various water matrices. A continuous-flow device utilizing MAC shows excellent performance in purifying micro-polluted water. Additionally, the degradation pathways of pollutants and changes in toxicity during the degradation process were identified through density functional theory (DFT) calculations, liquid chromatography-mass spectrometry (LC-MS), and toxicological analysis. Finally, the cultivation of green beans, peas, and wheat was found to significantly decrease the toxicity of contaminated water through degradation. This study proposes a low-cost method to enhance the activation pathway of non-radical PMS by utilizing modified activated carbon materials for pollutant remediation.

中文翻译：

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改性活性炭非自由基活化过一硫酸盐高效降解土霉素：机理与应用


由于其环境影响低、氧化剂用量温和，非均相非金属催化在非自由基过一硫酸盐（PMS）氧化中的应用具有重要意义。本研究的目的是使用酸改性活性炭和土霉素（OTC）作为代表性污染物来研究PMS的激活机制。改性活性炭 (MAC)/PMS 系统能够在 60 分钟内实现 100% 的 OTC 降解效率，观察到的速率常数 () 为 0.0414 分钟。 OTC 的降解主要是通过电子顺磁共振 (EPR) 和自由基猝灭研究介导的单线态氧 (O) 和电子转移过程中涉及的非自由基氧化途径。 PMS 的激活归因于 MAC 的结构缺陷、持久的自由基和氧官能团（如 C-OOH）。此外，MAC/PMS 系统始终能够在各种水基质中高效可靠地去除污染物。采用MAC的连续流装置在净化微污染水方面表现出优异的性能。此外，通过密度泛函理论（DFT）计算、液相色谱-质谱（LC-MS）和毒理学分析确定了污染物的降解途径和降解过程中毒性的变化。最后，人们发现种植青豆、豌豆和小麦可以通过降解显着降低受污染水的毒性。本研究提出了一种利用改性活性炭材料修复污染物的低成本方法来增强非自由基PMS的活化途径。