Activation of Oxygen and Hydrogen Peroxide by Copper(II) Coupled with Hydroxylamine for Oxidation of Organic Contaminants

被引:221
作者
Lee, Hongshin [1 ,3 ,4 ]
Lee, Hye-Jin [3 ,4 ]
Seo, Jiwon [3 ,4 ]
Kim, Hyung-Eun [3 ,4 ]
Shin, Yun Kyung [2 ]
Kim, Jae-Hong [1 ]
Lee, Changha [3 ,4 ]
机构
[1] Yale Univ, Dept Chem & Environm Engn, New Haven, CT 06511 USA
[2] NFRDI, Southeast Sea Fisheries Res Ctr, 397-68 Sanyangilju Ro, Tongyeong Si 53085, Gyeongsangnam D, South Korea
[3] UNIST, Sch Urban & Environm Engn, 50 UNIST Gil, Ulsan 44919, South Korea
[4] UNIST, KIST UNIST Ulsan Ctr Convergent Mat KUUC, 50 UNIST Gil, Ulsan 44919, South Korea
基金
新加坡国家研究基金会;
关键词
ZERO-VALENT IRON; CATALYZED DECOMPOSITION; RADICAL FORMATION; CIRCUMNEUTRAL PH; FENTON REACTION; ATOM TRANSFER; PHOTO-FENTON; FERROUS ION; WATER; KINETICS;
D O I
10.1021/acs.est.6b02067
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
This study reports that the combination of Cu(II) with hydroxylamine (HA) (referred to herein as Cu(II)/HA system) in situ generates H2O2 by reducing dissolved oxygen, subsequently producing reactive oxidants through the reaction of Cu(I) with H2O2. The external supply of H2O2 to the Cu(II)/HA system (i.e., the Cu(II)/H2O2/HA system) was found to further enhance the production of reactive oxidants. Both the Cu(II)/HA and Cu(II)/H2O2/HA. systems effectively oxidized benzoate (BA) at pH between 4 and 8, yielding a hydroxylated product, p-hydroxybenzoate (pHBA). The addition of a radical scavenger, tert-butyl alcohol, inhibited the BA oxidation in both systems. However, electron paramagnetic resonance (EPR) spectroscopy analysis indicated that (OH)-O-center dot was not produced under either acidic or neutral pH conditions, suggesting that the alternative oxidant, cupryl ion (Cu(III)), is likely a dominant oxidant.
引用
收藏
页码:8231 / 8238
页数:8
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