Constant oxidation of atrazine in Fe(III)/PDS system by enhancing Fe(III)/Fe(II) cycle with quinones: Reaction mechanism, degradation pathway and DFT calculation

化学 羟基自由基 对苯二酚 过氧二硫酸盐 羟基化 降级(电信) 氧化还原 核化学 光化学 激进的 环境化学 无机化学 有机化学 水溶液 电信 计算机科学
作者
Yujiao An,Xiaowan Li,Zihao Liu,Yiwen Li,Zhou Zhou,Xitao Liu
出处
期刊:Chemosphere [Elsevier]
卷期号:317: 137883-137883 被引量:25
标识
DOI:10.1016/j.chemosphere.2023.137883
摘要

Quinones are potential pollutants and redox active compounds widely distributed in environmental media. In this study, methyl-p-benzoquinone (MBQ) was introduced into Fe(III)/peroxydisulfate system (Fe(III)/PDS) to expedite the conversion of Fe(III) to Fe(II) and the degradation of atrazine (ATZ), ultimately establishing an environmentally friendly system of "treating pollution with pollution". MBQ/Fe(III)/PDS system showed superior performance to traditional Fe(II)/PDS system in pH range of 2-7. Sulfate radical (SO4•-) and hydroxyl radical (•OH) were confirmed to exist in MBQ/Fe(III)/PDS system according to alcohol quenching experiments and ESR tests. Meanwhile, stable 80% of η[PMSO2] (i.e., the molar ratio of PMSO2 generation to PMSO consumption) was achieved and manifested that highly reactive substance Fe(IV) also participated in MBQ/Fe(III)/PDS system. The spontaneous transformation of MBQ and methyl-hydroquinone (MHQ) drove Fe(III)/Fe(II) cycle, during which MHQ induced Fe(III) reduction and Fe(II) regeneration. Transformation pathways of ATZ were proposed based on HPLC-MS detection and DFT calculation and ATZ degradation could be initiated by lateral chain oxidation and dechlorination-hydroxylation. The acute toxicity, bioaccumulation factor, developmental toxicity and mutagenicity of ATZ and its degradation intermediates were evaluated by Toxicity Estimation Software Tool, and the luminescent bacteria test was conducted to investigate the acute toxicity variation of the reaction solution. Cl- obviously inhibited ATZ degradation and three main by-products generation, while humic acid (HA) had little effect on them probably due to the established balance between inhibition (some components in HA competed to consume reactive species) and acceleration (quinone units in HA also facilitated Fe(III)/Fe(II) cycle).
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