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Visible Light-Driven Selective Organic Degradation by FeTiO3/Persulfate System: the Formation and Effect of High Valent Fe(IV)
来源: | 作者:吴仕群 | 发布时间: 2021-01-29 | 735 次浏览 | 分享到:
Visible Light-Driven Selective Organic Degradation by FeTiO3/Persulfate System: the Formation and Effect of High Valent Fe(IV)
Lihan Pan†, Wen Shi†, Tapas Sen ‡, Lingzhi Wang†,*, Jinlong Zhang†,*
Abstract
The role of high-valent Fe has rarely been explored in persulfate-based heterogeneous reaction. Herein, the existence of Fe(IV) is verified in a visible light-assisted FeTiO3/persulfate system using methyl phenyl sulfoxide as the probe. The FeTiO3/persulfate/light system is capable of selectively degrading aromatic compounds with a higher ionization potential including tetracycline and bisphenol A by photo-generated high-valent Fe(IV). The contributions from SO4·- , ·OH and 1O2 are excluded. The comparable efficiency in the dark requires higher dosages and suffers from a rapid deactivation. Based on XPS, Raman and EPR analyses, the poor dark activity is caused by the formation of a complex between in situ formed Fe(III) and SO42- on the FeTiO3 surface; this complex is, however, the key intermediate for Fe(IV) production under the light irradiation. This study reveals the long-ignored role of SO42-  as an abundant species in iron-based persulfate systems. We also call for re-evaluating the real oxidation mechanism in other persulfate-based reactions considering the different oxidation mechanisms of radicals and high-valent iron.