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Novel FeII/EDDS/UV/PAA advanced oxidation process: Mechanisms and applications for naproxen degradation at neutral pH and low FeII dosage
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-12-01 , DOI: 10.1016/j.cej.2020.127896
Han Chen , Tao Lin , Shisheng Zhang , Hang Xu , Hui Tao , Wei Chen

The application of the integrated FeII/EDDS/UV/PAA (FEUP) process (EDDS = ethylenediamine-N,N’-disuccinic acid; PAA = peracetic acid) as a novel advanced oxidation process (AOP) for the degradation of a model contaminant, namely, naproxen (NAP), at neutral pH was investigated. The enhanced NAP degradation in this system at pH 7 was primarily attributable to the continuous activation of PAA via the UV-assisted FeII/FeIII cycle. A four-phase conceptual process of NAP degradation was established. The instantaneous degradation stage (IDS), in which FeII and PAA instantaneous react within 1 s, resulted in the degradation of ∼20% of NAP. The rapid degradation stage (RDS), in which the regenerated FeII rapidly activates PAA to produce the hydroxyl radicals (•OH) and organic radicals including CH3C(O)O•, CH3C(O)OO•, CH3OO• and •CH3 (defined as R-C•) without being scavenged by the FeII/FeIII-EDDS complexes, contributed to the degradation of ∼55% of NAP. The slow degradation stage (SDS), during which FeII/FeIII-EDDS complexes started competing for radicals, and resulted in the degradation of ∼15% of NAP. The continuous degradation stage (CDS), in which hydrogen peroxide (H2O2) was the only oxidant because PAA was exhausted, corresponded to the degradation of another ∼10% of NAP. The effect of water matrices including Cl-/Br-, HCO3-/CO32-, and humic acid (HA) was evaluated: Br-, HCO3-/CO32-, and HA exhibited an inhibiting effect on NAP degradation, while Cl- showed no influence on NAP degradation in the FEUP process. A superior degradation performance was achieved under a low FeII dosage and neutral conditions, demonstrating the great potential of the FEUP process for practical applications.



中文翻译:

新型Fe II / EDDS / UV / PAA高级氧化工艺:中性pH和低Fe II剂量下萘普生降解的机理和应用

集成的Fe II / EDDS / UV / PAA(FEUP)工艺(EDDS =乙二胺-N,N'-二丁二酸; PAA =过氧乙酸)作为一种新型的高级氧化工艺(AOP)用于模型降解研究了中性pH下的污染物,即萘普生(NAP)。在此系统中,pH 7时NAP降解的增强主要归因于通过UV辅助的Fe II / Fe III循环对PAA的连续活化。建立了NAP降解的四个阶段的概念过程。Fe II和PAA在1 s内瞬时反应的瞬时降解阶段(IDS)导致约20%的NAP降解。快速降解阶段(RDS),其中再生的Fe II快速活化PAA产生羟基自由基(•OH)和有机自由基,包括CH 3 C(O)O•,CH 3 C(O)OO•,CH 3 OO•和•CH 3(定义为RC•) Fe II / Fe III -EDDS络合物清除,导致了约55%的NAP降解。Fe II / Fe III -EDDS络合物开始竞争自由基的缓慢降解阶段(SDS),导致NAP降解约15%。连续降解阶段(CDS),其中过氧化氢(H 2 O 2)是唯一的氧化剂,因为PAA已耗尽,相当于另外约10%的NAP降解。水基质含Cl的效果- /溴-,HCO 3 - / CO 3 2-,和腐殖酸(HA)进行评价:溴-,HCO 3 - / CO 3 2-和HA显示对NAP具有抑制作用降解,而氯-显示在FEUP进程NAP降解没有影响。在低Fe II剂量和中性条件下获得了优异的降解性能,证明了FEUP工艺在实际应用中的巨大潜力。

更新日期:2020-12-01
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