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零价铁/H₂O₂/Fe²⁺体系中同时去除亚甲基蓝和总溶解铜:动力学、机制和降解途径。

Simultaneous removal of methylene blue and total dissolved copper in zero-valent iron/HO Fenton system: Kinetics, mechanism and degradation pathway.

机构信息

College of Architecture & Environment, Sichuan University, Chengdu 610065, China.

College of Architecture & Environment, Sichuan University, Chengdu 610065, China; Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06511, United States.

出版信息

J Colloid Interface Sci. 2019 Nov 1;555:383-393. doi: 10.1016/j.jcis.2019.07.071. Epub 2019 Jul 25.

DOI:10.1016/j.jcis.2019.07.071
PMID:31398566
Abstract

This study aimed to investigate the simultaneous removal of methylene blue (MB) and total dissolved copper (TCu) by heterogeneous zero-valent iron (ZVI) Fenton-like system (ZVI/HO) and elucidate the mechanism of synergistic effect for co-contaminants removal. Hydroxyl radical (OH) formation was hypothesized to be the dominant pathway for the oxidation of MB, confirmed by the quenching experiments and ESR analysis. And the synergistic effect of TCu and ZVI greatly promoted the release of Fe, further accelerating the generation of hydroxyl radical (OH) via Fenton reaction. The generation process of OH was unveiled by quenching experiments and electron spin resonance (ESR) analysis, while the processes of ZVI corrosion and TCu reduction were revealed through several characterization approaches including SEM, XRD, FTIR and XPS. The degradation pathway of MB was also investigated by LC-MS analysis. The MB initial concentration, TCu initial concentration, HO dosage, ZVI dosage and initial solution pH could play crucial roles in the removal of MB and TCu. The influence of water matrix including inorganic anions (Cl, NO, HCO) and actual water was finally conducted to elucidate the role of natural organic matter (NOM) in the environmental systems.

摘要

本研究旨在探讨非均相零价铁芬顿样体系(ZVI/HO)同时去除亚甲基蓝(MB)和总溶解铜(TCu),并阐明共污染物去除的协同作用机制。羟基自由基(OH)的形成被假设为 MB 氧化的主要途径,这通过猝灭实验和 ESR 分析得到了证实。并且 TCu 和 ZVI 的协同作用极大地促进了 Fe 的释放,通过芬顿反应进一步加速了羟基自由基(OH)的生成。通过猝灭实验和电子自旋共振(ESR)分析揭示了 OH 的生成过程,而通过 SEM、XRD、FTIR 和 XPS 等几种表征方法揭示了 ZVI 腐蚀和 TCu 还原的过程。还通过 LC-MS 分析研究了 MB 的降解途径。MB 的初始浓度、TCu 的初始浓度、HO 用量、ZVI 用量和初始溶液 pH 值在 MB 和 TCu 的去除中起着至关重要的作用。最后进行了水基质(包括无机阴离子(Cl、NO、HCO)和实际水)的影响研究,以阐明天然有机物(NOM)在环境系统中的作用。

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