Assessment of the Fe(III)-EDDS Complex in Fenton-Like Processes: From the Radical Formation to the Degradation of Bisphenol A

被引:336
作者
Huang, Wenyu [1 ,3 ]
Brigante, Marcello [1 ,2 ]
Wu, Feng [3 ]
Mousty, Christine [1 ,2 ]
Hanna, Khalil [4 ]
Mailhot, Gilles [1 ,2 ]
机构
[1] Clermont Univ, Univ Blaise Pascal ENSCCF, ICCF, F-63000 Clermont Ferrand, France
[2] CNRS, Inst Chim Clermont Ferrand, UMR 6296, F-63177 Aubiere, France
[3] Wuhan Univ, Sch Resources & Environm Sci, Dept Environm Sci, Wuhan 430079, Peoples R China
[4] Ecole Natl Super Chim Rennes UMR CNRS 6226 Sci Ch, CS 50837, F-35708 Rennes 7, France
基金
高等学校博士学科点专项科研基金;
关键词
HYDROGEN-PEROXIDE; AQUEOUS-SOLUTION; ACID; CHEMISTRY; MECHANISM; OXIDATION; IRON; DECOMPOSITION; REACTIVITY; HO2/O-2;
D O I
10.1021/es304502y
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The present work describes, for the first time, the use of a new and strong complexing agent, ethylenediamine-N,N'-disuccinic acid (EDDS) in the homogeneous Fenton process. The effect of H2O2 concentration, Fe(III)-EDDS concentration, pH value, and oxygen concentration on the homogeneous Fenton degradation of bisphenol A (BPA) used as a model pollutant, was investigated. Surprisingly, the performance of BPA oxidation in an EDDS-driven Fenton reaction was found to be much higher at near neutral or basic pH than at acidic pH. Inhibition and probe studies were conducted to ascertain the role of several radicals (e.g., (OH)-O-center dot, HO2 center dot/O-2(center dot-)) on BPA degradation. This unexpected effect of pH on Fenton reaction efficiency could be due to the formation of HO2 center dot or O-2(center dot-) radicals and to the presence of different forms of the complex Fe(III)-EDDS as a function of pH. Indeed, the reduction of Fe(III)-EDDS to Fe(II)-EDDS is a crucial step that governs the formation of hydroxyl radical, mainly responsible for BPA degradation. In addition to its ability to maintain iron in soluble form, EDDS acts as a superoxide radical-promoting agent, enhancing the generation of Fe(II) (the rate limiting step) and therefore the production of (OH)-O-center dot radicals. These results are very promising because they offer an important new treatment option at higher range of pH values and more particularly at pHs encountered in natural conditions.
引用
收藏
页码:1952 / 1959
页数:8
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