State Key Laboratory of Pollution Control and Resources Reuse, School of Environmental Science & Engineering, Tongji University, Shanghai, 200092, PR China; Shanghai Institute of Pollution Control and Ecological Security, 200092, Shanghai, PR China.
Department of Civil Engineering, The University of Hong Kong, 999077, Hong Kong, PR China.
J Hazard Mater. 2019 Mar 15;366:378-385. doi: 10.1016/j.jhazmat.2018.12.003. Epub 2018 Dec 3.
In this study, the presence of Cu(II) ions was found for the first time to severely inhibit +-dimethyl phthalate (DMP) degradation by ozone due to the formation of the stable complex Cu(II)-DMP. However, 100% DMP removal was rapidly reached when ethylenediamine tetraacetic acid (EDTA) was added with a Cu(II)/EDTA molar ratio of 3:1. Subsequent studies indicated that Cu(II)-DMP is sequestrated by EDTA, then DMP was degraded and Cu(II) was removed by precipitation. The freshly formed Cu-EDTA and organic nitrogen intermediates further decomposed O into OH, which induced to the rapid degradation of DMP. The k of Cu-EDTA/O were 9-10 times greater than the k of DMP removed by ozonation alone within 10 min. The reaction mechanism involved a OH generation was proposed. The OH and O- are generated from the rapid reaction between ozone and EDTA. Acting as a more strongly negative species, the specific Cu(II) in Cu-EDTA complexes is more inclined to react with O- to give Cu(I), accelerating the forward reaction to produce more OH. The synergistic removal of DMP and Cu(II) can be achieved after reaction. Therefore, this study provides an effective method to dispose metal ion and organic pollutant wastewater.
在这项研究中,首次发现 Cu(II) 离子的存在会严重抑制臭氧对邻苯二甲酸二甲酯(DMP)的降解,这是由于形成了稳定的配合物 Cu(II)-DMP。然而,当加入乙二胺四乙酸(EDTA)且 Cu(II)/EDTA 摩尔比为 3:1 时,DMP 可迅速达到 100%的去除率。随后的研究表明,Cu(II)-DMP 被 EDTA 螯合,然后 DMP 被降解,Cu(II) 通过沉淀去除。新形成的 Cu-EDTA 和有机氮中间体进一步将 O 分解为 OH,这导致 DMP 的快速降解。Cu-EDTA/O 的 k 值在 10 min 内比单独臭氧氧化去除 DMP 的 k 值高 9-10 倍。提出了一种涉及 OH 生成的反应机制。OH 和 O-是臭氧和 EDTA 之间快速反应生成的。作为一个带负电荷更强的物种,Cu-EDTA 配合物中的特定 Cu(II) 更倾向于与 O-反应生成 Cu(I),从而加速正向反应生成更多的 OH。反应后可以实现 DMP 和 Cu(II) 的协同去除。因此,本研究为处理金属离子和有机污染物废水提供了一种有效的方法。