Behavioral evidence of the dominant radicals and intermediates involved in Bisphenol A degradation using an efficient Co2+/PMS oxidation process

被引:165
作者
Huang, Yi-Fong [1 ]
Huang, Yao-Hui [1 ,2 ]
机构
[1] Natl Cheng Kung Univ, Dept Chem Engn, Tainan 701, Taiwan
[2] Natl Cheng Kung Univ, Sustainable Environm Res Ctr, Tainan 701, Taiwan
关键词
Endocrine disrupting chemicals; Bisphenol A; Peroxymonosulfate; Radicals; Mineralization; REACTIVE BLACK-B; PERSULFATE OXIDATION; AQUEOUS-SOLUTIONS; VISIBLE-LIGHT; ORANGE-II; MECHANISM; KINETICS; FENTON; WATER; ACTIVATION;
D O I
10.1016/j.jhazmat.2008.12.138
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 investigated the degradation and mineralization of Bisphenol A (BPA) at pH 7, taken as a model compound in the presence of the trace metal-ions, Co2+, and peroxymonosulfate (Oxone: PMS). We took advantage of the high oxidation-reduction potential of hydroxyl and sulfite radicals transformed from PMS as the oxidants to oxidize BPA to less complex compounds (stoichiometric ratio: [PMS](0)/[BPA](0) = 2). Afterwards, the expected radicals were used to mineralize those compounds more efficiently (TOC removal similar to 40%) as compared to the 1% removal demonstrated in the UV/persulfate system in our previous study. To the best of our knowledge, this is the first attempt to evidence that the dominant behavior of radicals in a (bi)sulfite process is very different from that in a persulfate process. Additionally, the utilization of extremely small amounts of activator and oxidant for the complete degradation of BPA was achieved. The BPA degradation in this Co2+/PMS process formulated a pseudo-first-order kinetic model well over a practicable range of 25-45 degrees C. The activation energy (Delta E = 57.6 kJ mol(-1)) was calculated under different conditions, and the detailed discussion indicates that the activity of BPA degradation is not obviously dependent on the PMS concentration, but rather is related to Co2+ dosage. Possible BPA side-chain oxidative metabolic pathways are suggested based on experimental results incorporating the evidence from EPR (electron paramagnetic resonance) and analysis from GC-MS (gas chromatography-mass spectrometry). (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:418 / 426
页数:9
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