Liang Chenju, Liang Ching-Ping, Chen Chi-Chin
Department of Environmental Engineering, National Chung Hsing University, 250 Kuo-kuang Road, Taichung 402, Taiwan.
J Contam Hydrol. 2009 May 12;106(3-4):173-82. doi: 10.1016/j.jconhyd.2009.02.008. Epub 2009 Feb 27.
The ability of free ferrous ion activated persulfate (S(2)O(8)(2-)) to generate sulfate radicals (SO(4)(-)) for the oxidation of trichloroethylene (TCE) is limited by the scavenging of SO(4)(-) with excess Fe(2+) and a quick conversion of Fe(2+) to Fe(3+). This study investigated the applicability of ethylene-diamine-tetra-acetic acid (EDTA) chelated Fe(3+) in activating persulfate for the destruction of TCE in aqueous phase under pH 3, 7 and 10. Fe(3+) and EDTA alone did not appreciably degrade persulfate. The presence of TCE in the EDTA/Fe(3+) activated persulfate system can induce faster persulfate and EDTA degradation due to iron recycling to activate persulfate under a higher pH condition. Increasing the pH leads to increases in pseudo-first-order-rate constants for TCE, S(2)O(8)(2-) and EDTA degradations, and Cl generation. Accordingly, the experiments at pH 10 with different EDTA/Fe(3+) molar ratios indicated that a 1/1 ratio resulted in a remarkably higher degradation rate at the early stage of reaction as compared to results by other ratios. Higher persulfate dosage under the EDTA/Fe(3+) molar ratio of 1/1 resulted in greater TCE degradation rates. However, increases in persulfate concentration may also lead to an increase in the rate of persulfate consumption.
游离亚铁离子活化过硫酸盐(S₂O₈²⁻)生成硫酸根自由基(SO₄⁻)以氧化三氯乙烯(TCE)的能力受到过量Fe²⁺对SO₄⁻的清除以及Fe²⁺快速转化为Fe³⁺的限制。本研究考察了乙二胺四乙酸(EDTA)螯合的Fe³⁺在pH值为3、7和10的水相中活化过硫酸盐以破坏TCE的适用性。单独的Fe³⁺和EDTA对过硫酸盐的降解作用不明显。在EDTA/Fe³⁺活化过硫酸盐体系中,TCE的存在可诱导过硫酸盐和EDTA更快降解,这是由于在较高pH条件下铁循环活化过硫酸盐所致。提高pH值会导致TCE、S₂O₈²⁻和EDTA降解以及Cl生成的准一级反应速率常数增加。因此,在pH为10时进行的不同EDTA/Fe³⁺摩尔比实验表明,与其他比例相比,1/1的比例在反应初期导致显著更高的降解速率。在EDTA/Fe³⁺摩尔比为1/1时,较高的过硫酸盐用量导致TCE降解速率更高。然而,过硫酸盐浓度的增加也可能导致过硫酸盐消耗速率增加。