Degradation of organic compounds during the corrosion of ZVI by hydrogen peroxide at neutral pH: Kinetics, mechanisms and effect of corrosion promoting and inhibiting ions

被引:65
|
作者
Ling, Ran [1 ]
Chen, J. Paul [1 ]
Shao, Jiahui [2 ]
Reinhard, Martin [3 ]
机构
[1] Natl Univ Singapore, Dept Civil & Environm Engn, 1 Engn Dr 2,E1A 07-03, Singapore 117576, Singapore
[2] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, 800 Dongchuan Rd, Shanghai 200240, Peoples R China
[3] Stanford Univ, Dept Civil & Environm Engn, Stanford, CA 94305 USA
基金
新加坡国家研究基金会;
关键词
Zero valent iron; Hydrogen peroxide; Fenton reaction; Corrosion; Hydroxyl radical; ZERO-VALENT IRON; ARTIFICIAL SWEETENERS; LOCALIZED CORROSION; METAL-IONS; OXIDATION; REMOVAL; DECOMPOSITION; PHOSPHATE; WATER; CONTAMINANTS;
D O I
10.1016/j.watres.2018.01.065
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The corrosion of zero valent iron (ZVI) by hydrogen peroxide (H2O2) generates hydroxyl (center dot OH) and other radical oxygen species (ROS) that degrade organic materials. To better understand the factors that govern the ROS formation during the. H2O2-induced corrosion, we investigated the degradation of an organic probe compound (acesulfame (ACE)) in slurries of ZVI powder in unbuffered laboratory water at pH 6.5 +/- 0.5. Chloride ions accelerated the corrosion of ZVI by H2O2 and the formation ROS and, therefore, the degradation of organic materials. Conversely, slowing corrosion by phosphate buffer inhibited ROS formation and the degradation of organic compounds. The rate of H2O2 decomposition was correlated with the liberation of Fe2+(aq) and the ACE degradation rate. The kinetics of H2O2 decomposition was pseudo-first-order and zero-order at low (<0.04 mMimg) and high [H2O2]/[ZVI] initial ratios, respectively, and was consistent with Langmuir kinetics. The H2O2 decomposition rate was proportional to the ZVI reactive surface area (SA) and nearly independent of the extent of ZVI oxidation, the presence of a Fe2+(aq) chelating agent, and center dot OH quenchers (methanol and tert-butanol). Kinetic data suggest a mechanism involving rapid cathodic reduction of H2O2 at the metallic ZVI surface which causes the liberation of Fe2+(aq) that generate center dot OH via the homogeneous Fenton reaction. The stoichiometric efficiency (SE) of organics degradation ranged from 0.0008% to 0.014% and increased with decreasing H2O2 decomposition rate. (C) 2018 Elsevier Ltd. All rights reserved.
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页码:44 / 53
页数:10
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