Phosphate Shifted Oxygen Reduction Pathway on Fe@Fe2O3 Core–Shell Nanowires for Enhanced Reactive Oxygen Species Generation and Aerobic 4-Chlorophenol Degradation,Environmental Science & Technology

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Phosphate Shifted Oxygen Reduction Pathway on Fe@Fe2O3 Core–Shell Nanowires for Enhanced Reactive Oxygen Species Generation and Aerobic 4-Chlorophenol Degradation
Environmental Science & Technology ( IF 10.8 ) Pub Date : 2017-07-05 00:00:00 , DOI: 10.1021/acs.est.7b01896
Yi Mu ₁ , Zhihui Ai ₁ , Lizhi Zhang ₁

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Phosphate ions widely exist in the environment. Previous studies revealed that the adsorption of phosphate ions on nanoscale zerovalent iron would generate a passivating oxide shell to block reactive sites and thus decrease the direct pollutant reduction reactivity of zerovalent iron. Given that molecular oxygen activation process is different from direct pollutant reduction with nanoscale zerovalent iron, it is still unclear how phosphate ions will affect molecular oxygen activation and reactive oxygen species generation with nanoscale zerovalent iron. In this study, we systematically studied the effect of phosphate ions on molecular oxygen activation with Fe@Fe₂O₃ nanowires, a special nanoscale zerovalent iron, taking advantages of rotating ring disk electrochemical analysis. It was interesting to find that the oxygen reduction pathway on Fe@Fe₂O₃ nanowires was gradually shifted from a four-electron reduction pathway to a sequential one-electron reduction one, along with increasing the phosphate ions concentration from 0 to 10 mmol·L^–1. This oxygen reduction pathway change greatly enhanced the molecular oxygen activation and reactive oxygen species generation performances of Fe@Fe₂O₃ nanowires, and thus increased their aerobic 4-chlorophenol degradation rate by 10 times. These findings shed insight into the possible roles of widely existed phosphate ions in molecular oxygen activation and organic pollutants degradation with nanoscale zerovalent iron.

中文翻译：

Fe @ Fe ₂ O ₃核壳纳米线上的磷酸转移氧还原途径可增强活性氧的产生和好氧4-氯苯酚的降解

磷酸盐离子广泛存在于环境中。先前的研究表明，磷酸根离子在纳米级零价铁上的吸附将产生钝化的氧化物壳，从而阻止反应位点，从而降低零价铁的直接污染物还原反应性。鉴于分子氧活化过程不同于采用纳米级零价铁的直接污染物还原，因此尚不清楚磷酸根离子将如何影响采用纳米级零价铁的分子氧活化和活性氧种类的产生。在这项研究中，我们系统地研究了磷酸根离子对Fe @ Fe ₂ O ₃对分子氧活化的影响。纳米线，一种特殊的纳米级零价铁，利用旋转环盘电化学分析的优势。有趣的是，Fe @ Fe ₂ O ₃纳米线上的氧还原途径逐渐从四电子还原途径转变为顺序的一电子还原途径，同时磷酸根离子浓度也从0增加到10 mmol· L ^–1。氧还原途径的改变极大地增强了Fe @ Fe ₂ O ₃的分子氧活化和活性氧的生成性能纳米线，因此将它们的好氧4-氯苯酚降解率提高了10倍。这些发现使人们深入了解了广泛存在的磷酸根离子在分子氧活化和纳米级零价铁降解有机污染物中的可能作用。

更新日期：2017-07-05

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