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Surface dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) for heterogeneous peroxymonosulfate activation to degrade diclofenac: Performance, mechanism and toxicity assessment
Journal of Hazardous Materials ( IF 13.6 ) Pub Date : 2020-11-18 , DOI: 10.1016/j.jhazmat.2020.124623
Junlei Zhang , Wei Zhao , Shanshan Wu , Renli Yin , Mingshan Zhu

Advanced oxidation processes (AOPs) based on heterogeneous catalytic activated peroxymonosulfate (PMS) have been becoming alternatives to conventional wastewater treatment technologies to directly degrade chemical contaminants. To build dual/multi redox cycles of different metal ions may be an effective means for better PMS activation. Herein, this study designed Mn3O4/CuBi2O4 with dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) to activate PMS for efficiently decomposing and mineralizing diclofenac sodium (DCF). Under optimal reaction conditions, DCF (50 mg/L) was degraded totally within 10 min, and TOC removal rate reached up to 74.3%. The possible mechanism of PMS activation by Mn3O4/CuBi2O4 was proposed, wherein dual redox cycles of Mn(III)/Mn(IV) and Cu(I)/Cu(II) on Mn3O4/CuBi2O4 effectively facilitated PMS activation to generate ·O2, 1O2, SO4· and ·OH, which was responsible for DCF degradation. Moreover, combined with degraded products detected by high resolution liquid chromatography coupled to mass spectrometry and corresponding toxic assessment results, the possible degradation pathways of DCF were proposed and the relative toxicity of degraded products was evaluated. This work may be useful for developing stronger heterogeneous activators of PMS to construct more efficient AOPs for purifying wastewater.



中文翻译:

Mn(III)/ Mn(IV)和Cu(I)/ Cu(II)的表面双氧化还原循环用于非均相过氧单硫酸盐活化以降解双氯芬酸:性能,机理和毒性评估

基于非均相催化活化过氧单硫酸盐(PMS)的高级氧化工艺(AOP)已成为传统废水处理技术的替代品,以直接降解化学污染物。建立不同金属离子的双重/多重氧化还原循环可能是更好地激活PMS的有效手段。在此,本研究设计了具有Mn(III)/ Mn(IV)和Cu(I)/ Cu(II)双重氧化还原循环的Mn 3 O 4 / CuBi 2 O 4来激活PMS,以有效地分解和矿化双氯芬酸钠(DCF)。 )。在最佳反应条件下,DCF(50 mg / L)在10分钟内完全降解,TOC去除率达到74.3%。Mn 3 O 4激活PMS的可能机理提出了/ CuBi 2 O 4,其中Mn 3 O 4 / CuBi 2 O 4上的Mn(III)/ Mn(IV)和Cu(I)/ Cu(II)的双重氧化还原循环有效地促进了PMS活化以生成· O 2 1 O 2,SO 4 · ·OH,这是DCF降解的原因。此外,结合高分辨率液相色谱-质谱联用法检测到的降解产物以及相应的毒性评估结果,提出了DCF可能的降解途径,并对降解产物的相对毒性进行了评价。这项工作可能有助于开发更强大的PMS异质活化剂,以构建更有效的AOP来净化废水。

更新日期:2020-11-18
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