Katsenovich Yelena P, Miralles-Wilhelm Fernando R
Applied Research Center, Florida International University, 10555 W. Flagler St., Suite 2100, Miami, FL, 33174, United States.
Sci Total Environ. 2009 Sep 1;407(18):4986-93. doi: 10.1016/j.scitotenv.2009.05.033. Epub 2009 Jun 30.
The longevity and reactivity of nanoscale zerovalent iron (nZVI) and palladized bimetallic particles (BNP) were evaluated in batch and column experiments for remediation of a trichloroethene (TCE)-contaminated plume within a clayey soil from Oak Ridge Reservation (ORR). Comparative studies assessing the viability of BNP and nZVI confirmed that particle behavior is severely affected by clay sediments. Surface morphology and composition analyses using SEM and SEM-energy-dispersive spectroscopy spectrum revealed particle agglomeration through the formation of clay-iron aggregates of greater mass during the early phase of the experiment. Batch study results suggest that TCE degradation in ORR clayey soil follows a pseudo-first-order kinetic model exhibiting reaction rate constants (k) of 0.05-0.24 day(-1) at varied iron-to-soil ratios. Despite high reactivity in water, BNP were less effective in the site-derived clay sediment with calculated TCE removal efficiencies of 98.7% and 19.59%, respectively. A column experiment was conducted to investigate particle longevity and indicator parameters of the TCE degradation process under flow conditions. It revealed that the TCE removal efficiency gradually declined over the course of the experiment from 86-93% to 51-52%, correlating to a progressive increase in oxidation-reduction potential (ORP) from -485 to -250 mV and pH drop from 8.2-8.6 to 7.4-7.5. The rate of nZVI deactivation reaction was found to be a first order with a k(d) value of 0.0058 day(-1). SEM images of residual nZVI revealed heavily agglomerated particles. However, despite widespread oxidation and agglomeration, particles managed to maintain some capacity for oxidation. A quantitative analysis of nZVI deactivation has the potential of predicting nZVI longevity in order to improve the design strategy of TCE remediation.
在批量实验和柱实验中评估了纳米零价铁(nZVI)和钯化双金属颗粒(BNP)的寿命和反应活性,以修复来自橡树岭国家实验室(ORR)的受三氯乙烯(TCE)污染的粘性土壤中的羽状污染物。评估BNP和nZVI可行性的对比研究证实,颗粒行为受到粘土沉积物的严重影响。使用扫描电子显微镜(SEM)和SEM能量色散光谱对表面形态和成分进行分析,结果显示,在实验初期,通过形成质量更大的粘土-铁聚集体,颗粒发生了团聚。批量研究结果表明,ORR粘性土壤中TCE的降解遵循准一级动力学模型,在不同的铁与土壤比例下,反应速率常数(k)为0.05-0.24天-1。尽管BNP在水中具有高反应活性,但在源自现场的粘土沉积物中效果较差,计算得出的TCE去除效率分别为98.7%和19.59%。进行了柱实验,以研究流动条件下颗粒寿命和TCE降解过程的指示参数。结果表明,在实验过程中,TCE去除效率从86-93%逐渐下降至51-52%,这与氧化还原电位(ORP)从-485 mV逐渐升高至-250 mV以及pH从8.2-8.6下降至7.4-7.5相关。发现nZVI失活反应速率为一级反应,k(d)值为0.0058天-1。残留nZVI的SEM图像显示颗粒严重团聚。然而,尽管发生了广泛的氧化和团聚,颗粒仍保持了一定的氧化能力。对nZVI失活进行定量分析有潜力预测nZVI的寿命,从而改进TCE修复的设计策略。