College of Chemical Engineering, Huaqiao University, Xiamen, 361021, China.
Environ Sci Pollut Res Int. 2019 Aug;26(24):24707-24719. doi: 10.1007/s11356-019-05601-4. Epub 2019 Jun 25.
Efficient abatement of an iodinated X-ray contrast media iohexol by an emerging sulfite autoxidation advanced oxidation process is demonstrated, which is based on transition metal ion-catalyzed autoxidation of sulfite to form active oxidizing species. The efficacy of the combination of sulfite and transition metal ions (Ag(I), Mn(II), Co(II), Fe(II), Cu(II), Fe(III), or Ce(III)) was tested for iohexol abatement. Co(II) and Cu(II) are proven to show more pronounced catalytic activity than other metals at pH 8.0. According to the quenching studies, sulfate radical (SO) is identified to be the primary species for oxidation of iohexol. Increasing dosages of metal ion or sulfite and higher pH values are favorable for iohexol abatement. Inhibition of iohexol abatement is observed in the absence of dissolved oxygen, which is vital for the production of SO and subsequent formation of SO. Overall, activation of sulfite to produce reactive radicals with extremely low Co(II) or Cu(II) concentrations (in the range of μg L) in circumneutral conditions is confirmed, which offers a potential SO-based advanced oxidation process in treatment of aquatic organic contaminants.
基于过渡金属离子催化亚硫酸盐自氧化形成活性氧化物种,本研究展示了一种新兴的亚硫酸盐自氧化高级氧化工艺可有效去除碘造影剂碘海醇。测试了亚硫酸盐与过渡金属离子(Ag(I)、Mn(II)、Co(II)、Fe(II)、Cu(II)、Fe(III)或 Ce(III))的组合对碘海醇去除的效果。结果表明,在 pH 8.0 时,Co(II)和 Cu(II)比其他金属表现出更显著的催化活性。根据猝灭实验的结果,鉴定出硫酸盐自由基(SO)是氧化碘海醇的主要物质。增加金属离子或亚硫酸盐的剂量以及提高 pH 值有利于碘海醇的去除。在没有溶解氧的情况下,观察到碘海醇的去除受到抑制,这对于 SO 的产生和随后的 SO 形成至关重要。总之,在近中性条件下,确认了在非常低的 Co(II)或 Cu(II)浓度(μg/L 范围内)下激活亚硫酸盐以产生具有高反应活性的自由基,这为基于 SO 的高级氧化工艺处理水相有机污染物提供了一种潜在的方法。