College of Architecture & Environment, Sichuan University, Chengdu 610065, China.
College of Architecture & Environment, Sichuan University, Chengdu 610065, China; Sino-German Centre for Water and Health Research, Sichuan University, Chengdu 610065, China.
Sci Total Environ. 2021 Nov 25;797:149097. doi: 10.1016/j.scitotenv.2021.149097. Epub 2021 Jul 17.
Slow reduction of Fe(III) in iron-mediated Fenton-like systems strongly limits the decomposition of HO to produce hydroxyl radicals (OH). Here, we report that graphene oxide (GO) possesses excellent reactivity to enhance the Fe(III)/HO Fenton and photo-Fenton oxidation for degrading chloramphenicol (CAP). EPR analysis and quenching tests reveal that OH is the primary oxidant for CAP degradation. The characterization analysis and iron species transformation experiments demonstrate that Fe(III) can combine with the functional groups on the GO surface to form GO-Fe(III) complexes. The chronopotentiometry and cyclic voltammogram suggest that GO can donate electrons to Fe(III) via intramolecular electron transfer and promote HO induced Fe(III) reduction by increasing the oxidation capability of Fe(III) due to the formation of GO-Fe(III) complexes, resulting in the strong promotion of the Fe(III)/Fe(II) cycle for producing OH. Moreover, the dark- and vis-GO/Fe(III)/HO systems can effectively degrade CAP at initial pH ranging from 2.0 to 4.7. The reusability and stability of GO were evaluated by performing the cyclic degradation experiments of CAP. The OH induced degradation pathway of CAP was proposed involving three stages, based on intermediates analysis of UPLC-QTOF-MS/MS system. Therefore, the GO/Fe(III)/HO system with or without visible light shows high potential for application in environmental remediation.
铁介导的类芬顿体系中 Fe(III) 的缓慢还原强烈限制了 HO 的分解以产生羟基自由基 (OH)。在这里,我们报告氧化石墨烯 (GO) 具有优异的反应性,可增强 Fe(III)/HO 芬顿和光芬顿氧化,以降解氯霉素 (CAP)。EPR 分析和猝灭实验表明,OH 是 CAP 降解的主要氧化剂。表征分析和铁物种转化实验表明,Fe(III) 可以与 GO 表面的官能团结合形成 GO-Fe(III) 配合物。恒电流计时和循环伏安法表明,GO 可以通过分子内电子转移将电子供体给 Fe(III),并由于形成 GO-Fe(III) 配合物而增加 Fe(III)的氧化能力,从而促进 HO 诱导的 Fe(III)还原,导致 Fe(III)/Fe(II) 循环强烈促进 OH 的产生。此外,暗和可见光 GO/Fe(III)/HO 体系可以在初始 pH 值为 2.0 至 4.7 的范围内有效降解 CAP。通过进行 CAP 的循环降解实验评估了 GO 的可重复使用性和稳定性。根据 UPLC-QTOF-MS/MS 系统的中间产物分析,提出了 CAP 被 OH 诱导降解的途径,涉及三个阶段。因此,具有或不具有可见光的 GO/Fe(III)/HO 体系在环境修复中具有很高的应用潜力。