College of Chemical Engineering, Huaqiao University, Xiamen 361021, China.
College of Chemical Engineering, Huaqiao University, Xiamen 361021, China.
Sci Total Environ. 2019 Dec 10;695:133836. doi: 10.1016/j.scitotenv.2019.133836. Epub 2019 Aug 7.
Sulfite has been recently emerging as an appealing sulfate radical (SO) precursor for efficient treatment of organic contaminants. Due to the negligible autoxidation of sulfite, activators are often introduced to accelerate sulfite autoxidation and the concomitant generation of SO. Present heterogeneous activators are mostly not very effective under mild conditions (pH 7.0-8.0). In this work, efficient activation of sulfite with copper oxides including CuO and CuO for iohexol degradation under mild pH conditions is proposed. In a comparison of iohexol degradation efficiency by sulfite autoxidation activated with different metal oxides (CoO, CoO, α-FeO, γ-FeO, CuO and CuO), CuO and CuO with lower toxicity are efficient activators and removal efficiencies of ~95% can be obtained at pH 8.0. SO is identified to be the major species contributing to the removal of iohexol by electron paramagnetic resonance (EPR) spectroscopy and quenching experiment. Based on the effect of ionic strength and copper leaching, sulfite is proposed to interact with copper oxides via inner-sphere coordination. Effect of critical influencing parameters and efficacy of copper oxides in real water matrixes are investigated. The results suggest that using copper oxides as activators is a new alternative to promote sulfite autoxidation process for rapid contaminants degradation.
亚硫酸盐最近作为一种有吸引力的硫酸根自由基 (SO) 前体而出现,可有效处理有机污染物。由于亚硫酸盐的自氧化作用可以忽略不计,因此通常引入活化剂来加速亚硫酸盐的自氧化和伴随的 SO 的生成。目前的多相活化剂在温和条件下(pH 值 7.0-8.0)大多不是非常有效。在这项工作中,提出了在温和 pH 条件下使用氧化铜(包括 CuO 和 CuO)有效激活亚硫酸盐以降解碘海醇。在比较不同金属氧化物(CoO、CoO、α-FeO、γ-FeO、CuO 和 CuO)活化的亚硫酸盐自氧化对碘海醇降解效率的实验中,毒性较低的 CuO 和 CuO 是有效的活化剂,在 pH 值为 8.0 时可以获得约 95%的去除效率。电子顺磁共振(EPR)光谱和猝灭实验表明,SO 是去除碘海醇的主要物质。基于离子强度的影响和铜浸出的实验结果,亚硫酸盐被提出通过内球配位与氧化铜相互作用。还考察了关键影响参数和铜氧化物在实际水基质中的功效。结果表明,使用铜氧化物作为活化剂是促进亚硫酸盐自氧化过程以快速降解污染物的一种新选择。