Choi Hyeok, Agarwal Shirish, Al-Abed Souhail R
National Risk Management Research Laboratory, U.S. Environmental Protection Agency, 26 West Martin Luther King Drive, Cincinnati, Ohio 45268, USA.
Environ Sci Technol. 2009 Jan 15;43(2):488-93. doi: 10.1021/es8015815.
There are many concerns and challenges in current remediation strategies for sediments contaminated with polychlorinated biphenyls (PCBs). Our efforts have been geared toward the development of granular activated carbon (GAC) impregnated with reactive iron/palladium (Fe/Pd) bimetallic nanoparticles (reactive activated carbon (RAC)). In this study, we elucidate the mechanistic aspects of the hybrid RAC system dechlorinating 2-chlorobiphenyl (2-CIBP) in the aqueous phase. The following reactions occurred in parallel or consecutively: (i) 2-CIBP is promptly and completely sequestrated to RAC phase, (ii) the adsorbed 2-CIBP is almost simultaneously dechlorinated by Fe/Pd particles to form a reaction product biphenyl (BP), and (iii) the BP formed is instantly and strongly adsorbed to RAC. The 2-CIBP adsorption and dechlorination rate constants were estimated through simple first-order reaction kinetic models with an assumption for unextractable portion of carbon in RAC. The extent of 2-CIBP accumulation and BP formation in RAC phase could be well explained by the kinetic model and adsorption was found to be the rate limiting step for overall reaction. On the basis of our observations, a new strategy and concept of "reactive" cap/barrier composed of RAC was proposed as a new environmental risk management option for PCBs-contaminated sites.
目前,针对多氯联苯(PCBs)污染沉积物的修复策略存在诸多问题与挑战。我们致力于开发负载有活性铁/钯(Fe/Pd)双金属纳米颗粒的颗粒活性炭(GAC),即反应性活性炭(RAC)。在本研究中,我们阐明了RAC混合体系在水相中对2-氯联苯(2-CIBP)进行脱氯的机理。发生了以下平行或连续反应:(i)2-CIBP迅速且完全被螯合到RAC相中;(ii)吸附的2-CIBP几乎同时被Fe/Pd颗粒脱氯,形成反应产物联苯(BP);(iii)生成的BP立即并强烈吸附到RAC上。通过简单的一级反应动力学模型,在假设RAC中碳不可萃取部分的情况下,估算了2-CIBP的吸附和脱氯速率常数。动力学模型能够很好地解释RAC相中2-CIBP的积累程度和BP的形成,并且发现吸附是整个反应的速率限制步骤。基于我们的观察结果,提出了一种由RAC组成的“反应性”覆盖层/屏障的新策略和概念,作为受PCBs污染场地的一种新的环境风险管理选项。