Ayoung Choi, Changseok Han, Eric Lichtfouse, Virender K. Sharma
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Batch experiments were conducted under with and without ultraviolet irradiation at nearly neutral pH with varying peroxyacetic acid concentrations. The reaction of 6PPD-Q with peroxyacetic acid promoted radical amplification via electron transfer and semiquinone radicals formation, enabling 6PPD-Q degradation with more than 70% removal at 65 µM peroxyacetic acid, and complete degradation within 60 min at 263 µM peroxyacetic acid. Ultraviolet irradiation, while not required for semiquinone radical formation, enhanced overall degradation by promoting additional radical generation. 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引用次数: 0
摘要
N -(1,3-二甲基丁基)- N′-苯基-对苯二胺(6PPD)及其臭氧化产物6PPD-醌(6PPD- q)因其广泛存在和对水生生物的急性毒性而受到全球关注。常规的处理方法往往不能将其在水中完全去除。过氧乙酸广泛用于高级氧化工艺;然而,它通常依赖于紫外线照射来产生活性自由基。在这里,我们首次证明了目标污染物6PPD-Q与过氧乙酸发生反应,促进自由基扩增,并在没有外部能量输入的情况下诱导其自身降解。在接近中性的pH值和不同的过氧乙酸浓度下,在有和无紫外线照射下进行了批量实验。6PPD-Q与过氧乙酸的反应促进了自由基通过电子转移扩增和半醌自由基的形成,在65µM过氧乙酸条件下6PPD-Q的去除率超过70%,在263µM过氧乙酸条件下60 min内完全降解。紫外线照射虽然不是半醌自由基形成所必需的,但通过促进额外自由基的产生,增强了整体降解。总的来说,我们提供了污染物驱动的过氧乙酸活化和自由基扩增的第一个证据,为醌介导的氧化剂活化和醌衍生污染物的无催化剂修复策略提供了新的见解。
Self-destruction of a tire-derived quinone pollutant by peroxyacetic acid
N -(1,3-Dimethylbutyl)- N '-phenyl- p -phenylenediamine (6PPD) and its ozonation product, 6PPD-quinone (6PPD-Q), are contaminants of global concern due to their widespread occurrence and acute toxicity to aquatic organisms. Conventional treatment methods often fail to its complete removal in water. Peroxyacetic acid is extensively employed in advanced oxidation processes; however, it relies generally on ultraviolet light irradiation to generate reactive radical species. Here, we demonstrate for the first time that the target pollutant 6PPD-Q reacted with peroxyacetic acid to promote radical amplification and induced its own degradation without external energy input. Batch experiments were conducted under with and without ultraviolet irradiation at nearly neutral pH with varying peroxyacetic acid concentrations. The reaction of 6PPD-Q with peroxyacetic acid promoted radical amplification via electron transfer and semiquinone radicals formation, enabling 6PPD-Q degradation with more than 70% removal at 65 µM peroxyacetic acid, and complete degradation within 60 min at 263 µM peroxyacetic acid. Ultraviolet irradiation, while not required for semiquinone radical formation, enhanced overall degradation by promoting additional radical generation. Overbally, we provide the first evidence of pollutant-driven peroxyacetic acid activation and radical amplification, offering new insight into quinone-mediated oxidant activation and a catalyst-free remediation strategy for quinone-derived contaminants.
期刊介绍:
Environmental Chemistry Letters explores the intersections of geology, chemistry, physics, and biology. Published articles are of paramount importance to the examination of both natural and engineered environments. The journal features original and review articles of exceptional significance, encompassing topics such as the characterization of natural and impacted environments, the behavior, prevention, treatment, and control of mineral, organic, and radioactive pollutants. It also delves into interfacial studies involving diverse media like soil, sediment, water, air, organisms, and food. Additionally, the journal covers green chemistry, environmentally friendly synthetic pathways, alternative fuels, ecotoxicology, risk assessment, environmental processes and modeling, environmental technologies, remediation and control, and environmental analytical chemistry using biomolecular tools and tracers.