Lee Woojin, Batchelor Bill
Environment and Process Technology Division, Korea Institute of Science and Technology, P.O. Box 131, Cheongryang, Seoul 130-650, South Korea.
Chemosphere. 2004 Sep;56(10):999-1009. doi: 10.1016/j.chemosphere.2004.05.015.
Abiotic reductive dechlorination of chlorinated ethylenes (tetrachloroethylene (PCE), trichloroethylene (TCE), cis-dichloroethylene (c-DCE), and vinylchloride (VC)) by iron-bearing phyllosilicates (biotite, vermiculite, and montmorillonite) was characterized to obtain better understanding of the behavior of these contaminants in systems undergoing remediation by natural attenuation and redox manipulation. Batch experiments were conducted to evaluate dechlorination kinetics and some experiments were conducted with addition of Fe(II) to simulate impact of microbial iron reduction. A modified Langmuir-Hinshelwood kinetic model adequately described reductive dechlorination kinetics of target organics by the iron-bearing phyllosilicates. The rate constants stayed between 0.08 (+/-10.4%) and 0.401 (+/-8.1%) day(-1) and the specific initial reductive capacity of iron-bearing phyllosilicates for chlorinated ethylenes stayed between 0.177 (+/-6.1%) and 1.06 (+/-7.1%) microM g(-1). The rate constants for the reductive dechlorination of TCE at reactive biotite surface increased as pH (5.5-8.5) and concentration of sorbed Fe(II) (0-0.15 mM g(-1)) increased. The appropriateness of the model is supported by the fact that the rate constants were independent of solid concentration (0.0085-0.17 g g(-1)) and initial TCE concentration (0.15-0.60 mM). Biotite had the greatest rate constant among the phyllosilicates both with and without Fe(II) addition. The rate constants were increased by a factor of 1.4-2.5 by Fe(II) addition. Between 1.8% and 36% of chlorinated ethylenes removed were partitioned to the phyllosilicates. Chloride was produced as a product of degradation and no chlorinated intermediates were observed throughout the experiment.
通过含铁层状硅酸盐(黑云母、蛭石和蒙脱石)对氯化乙烯(四氯乙烯(PCE)、三氯乙烯(TCE)、顺式二氯乙烯(c-DCE)和氯乙烯(VC))进行非生物还原脱氯,以更好地了解这些污染物在通过自然衰减和氧化还原操纵进行修复的系统中的行为。进行了批次实验以评估脱氯动力学,并进行了一些添加Fe(II)的实验以模拟微生物铁还原的影响。修正的Langmuir-Hinshelwood动力学模型充分描述了含铁层状硅酸盐对目标有机物的还原脱氯动力学。速率常数介于0.08(±10.4%)和0.401(±8.1%)天⁻¹之间,含铁层状硅酸盐对氯化乙烯的比初始还原容量介于0.177(±6.1%)和1.06(±7.1%)微摩尔克⁻¹之间。在活性黑云母表面,TCE还原脱氯的速率常数随pH值(5.5 - 8.5)和吸附的Fe(II)浓度(0 - 0.15毫摩尔克⁻¹)的增加而增加。该模型的适用性得到以下事实的支持:速率常数与固体浓度(0.0085 - 0.17克克⁻¹)和初始TCE浓度(0.15 - 0.60毫摩尔)无关。在添加和不添加Fe(II)的层状硅酸盐中,黑云母的速率常数最大。添加Fe(II)后,速率常数增加了1.4 - 2.5倍。去除的氯化乙烯中有1.8%至36%分配到层状硅酸盐中。降解产物为氯离子,整个实验过程中未观察到氯化中间体。