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为什么多途径协同作用(如 PMS 系统中的激进和非激进途径)比单途径在四环素降解中具有更高的效率。

Why the cooperation of radical and non-radical pathways in PMS system leads to a higher efficiency than a single pathway in tetracycline degradation.

机构信息

State Key Lab of Urban Water Resource and Environment, School of Civil and Environmental Engineering, Harbin Institute of Technology Shenzhen, Shenzhen 518055, PR China; School of Civil and Environmental Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen, Guangdong 518055, PR China.

State Key Lab of Urban Water Resource and Environment, School of Civil and Environmental Engineering, Harbin Institute of Technology Shenzhen, Shenzhen 518055, PR China; School of Civil and Environmental Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen, Guangdong 518055, PR China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt A):127247. doi: 10.1016/j.jhazmat.2021.127247. Epub 2021 Sep 20.

Abstract

Current research focused on developing multiple active species in peroxymonosulfate (PMS) system to degrade contaminants, but deepening concern lacks over why cooperation of those active species facilitated a faster degradation. Here, we employed CoO, rGO and CoO@rGO composite to activate PMS for tetracycline (TC) degradation, and detected crucial factors toward highest performance of CoO@rGO/PMS system. Batch experiments exhibited a satisfactory TC degradation efficiency under CoO@rGO/PMS, complete degraded 50 mg/L TC within 20 min. Analytical tests discovered that radical active species generated by CoO/PMS and non-radical species by rGO/PMS were successfully co-existed in CoO@rGO/PMS system, significantly improving the performance of TC removal. Subsequently, a combination of density functional theory (DFT) calculation and intermediates analysis revealed that, in CoO@rGO/PMS system, the cooperation rather than independent effect of radical and non-radical active species expanded TC degradation pathways, enhancing the degradation performance. Furthermore, decent adaptability, stability, and recyclability toward affecting factors variation of CoO@rGO/PMS demonstrated it as a potent and economical system to degrade TC. Overall, this study developed a novel CoO@rGO/PMS system with a cooperative oxidation pathway for highly efficient TC removal, and managed to clarify why this oxidation pathway achieved high efficiency through a combination of theoretical and experimental method.

摘要

目前的研究集中在开发过一硫酸氢盐(PMS)体系中的多种活性物种来降解污染物,但对于为什么这些活性物种的合作促进了更快的降解,人们的关注还不够深入。在这里,我们采用 CoO、rGO 和 CoO@rGO 复合材料来激活 PMS 降解四环素(TC),并检测了 CoO@rGO/PMS 体系中达到最高性能的关键因素。批量实验表明,在 CoO@rGO/PMS 下,TC 具有令人满意的降解效率,在 20 分钟内完全降解了 50mg/L 的 TC。分析测试发现,CoO/PMS 产生的自由基活性物种和 rGO/PMS 产生的非自由基活性物种在 CoO@rGO/PMS 体系中成功共存,显著提高了 TC 去除性能。随后,通过密度泛函理论(DFT)计算和中间体分析相结合的方法揭示,在 CoO@rGO/PMS 体系中,自由基和非自由基活性物种的协同作用而非独立作用扩展了 TC 降解途径,增强了降解性能。此外,CoO@rGO/PMS 对影响因素变化具有良好的适应性、稳定性和可回收性,证明其是一种高效去除 TC 的有效且经济的体系。总的来说,本研究开发了一种新型的 CoO@rGO/PMS 协同氧化途径体系,用于高效去除 TC,并通过理论和实验相结合的方法阐明了为什么这种氧化途径能够达到高效。

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