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中性 pH 下 Cu(II)催化芬顿样反应增强氯离子氧化有机污染物。

Chloride-enhanced oxidation of organic contaminants by Cu(II)-catalyzed Fenton-like reaction at neutral pH.

机构信息

School of Urban and Environmental Engineering, Ulsan National Institute of Science and Technology (UNIST), 50 UNIST-gil, Ulju-gun, Ulsan 44919, Republic of Korea.

Department of Chemical and Environmental Engineering, Yale University, New Haven, Connecticut 06511, USA.

出版信息

J Hazard Mater. 2018 Feb 15;344:1174-1180. doi: 10.1016/j.jhazmat.2017.10.020. Epub 2017 Oct 12.

Abstract

The Cu(II)-catalyzed Fenton-like reaction was found to be significantly accelerated in the presence of chloride ion (i.e., the Cu(II)/HO/Cl system), enhancing the oxidative degradation of organic contaminants at neutral pH. The degradation of carbamazepine (a select target contaminant) by the Cu(II)/HO system using 1μM Cu(II) and 10mM HO was accelerated by 28-fold in the presence of 10,000mg/L Cl at pH 7. The observed rate of carbamazepine degradation generally increased with increasing doses of Cu(II), HO, and Cl, and exhibited an optimal value at around pH 7.5. Various other organic contaminants such as propranolol, phenol, acetaminophen, 4-chlorophenol, benzoic acid, and caffeine were also effectively degraded by the Cu(II)/HO/Cl system. Experiments using oxidant probe compounds and electron paramagnetic spectroscopy suggested that cupryl (Cu(III)) species are the major reactive oxidants responsible for the degradation of these organic contaminants. The enhanced kinetics was further confirmed in natural seawater.

摘要

在氯离子(即 Cu(II)/HO/Cl 体系)存在下,发现 Cu(II)催化的类芬顿反应显著加速,增强了中性 pH 下有机污染物的氧化降解。在 pH 7 时,10,000mg/L Cl 的存在下,用 1μM Cu(II)和 10mM HO 的 Cu(II)/HO 体系使卡马西平(一种选择的目标污染物)的降解速度加快了 28 倍。卡马西平降解的观察速率通常随 Cu(II)、HO 和 Cl 的剂量增加而增加,并在 pH 7.5 左右呈现最佳值。其他各种有机污染物,如普萘洛尔、苯酚、对乙酰氨基酚、4-氯苯酚、苯甲酸和咖啡因,也被 Cu(II)/HO/Cl 体系有效降解。使用氧化剂探针化合物和电子顺磁共振波谱实验表明,铜酰(Cu(III))物种是导致这些有机污染物降解的主要反应性氧化剂。在天然海水中进一步证实了增强的动力学。

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