Slater G F, Lollar B Sherwood, King R Allen, O'Hannesin S
Department of Marine Chemistry and Geochemistry, Woods Hole Oceanographic Institution, MA 02543-1543, USA.
Chemosphere. 2002 Nov;49(6):587-96. doi: 10.1016/s0045-6535(02)00327-2.
During reductive dechlorination of trichloroethene (TCE) by zero-valent iron, stable carbon isotopic values of residual TCE fractionate significantly and can be described by a Rayleigh model. This study investigated the effect of observed reaction rate, surface oxidation and iron type on isotopic fractionation of TCE during reductive dechlorination. Variation of observed reaction rate did not produce significant differences in isotopic fractionation in degradation experiments. However, a small influence on isotopic fractionation was observed for experiments using acid-cleaned electrolytic iron versus experiments using autoclaved electrolytic iron, acid-cleaned Peerless cast iron or autoclaved Peerless cast iron. A consistent isotopic enrichment factor of epsilon = -16.7/1000 was determined for all experiments using cast iron, and for the experiments with autoclaved electrolytic iron. Column experiments using 100% cast iron and a 28% cast iron/72% aquifer matrix mixture also resulted in an enrichment factor of -16.9/1000. The consistency in enrichment factors between batch and column systems suggests that isotopic trends observed in batch systems may be extrapolated to flowing systems such as field sites. The fact that significant isotopic fractionation was observed in all experiments implies that isotopic analysis can provide a direct qualitative indication of whether or not reductive dechlorination of TCE by Fe0 is occurring. This evidence may be useful in answering questions which arise at field sites, such as determining whether TCE observed down-gradient of an iron wall remediation scheme is the result of incomplete degradation within the wall, or of the dissolved TCE plume by passing the wall.
在零价铁对三氯乙烯(TCE)进行还原脱氯过程中,残留TCE部分的稳定碳同位素值会发生显著分馏,且可用瑞利模型来描述。本研究调查了观察到的反应速率、表面氧化和铁的类型对TCE还原脱氯过程中同位素分馏的影响。在降解实验中,观察到的反应速率变化并未在同位素分馏方面产生显著差异。然而,与使用经酸清洗的电解铁、经高压灭菌的电解铁、经酸清洗的Peerless铸铁或经高压灭菌的Peerless铸铁的实验相比,使用经酸清洗的电解铁的实验对同位素分馏有较小影响。对于所有使用铸铁的实验以及使用经高压灭菌的电解铁的实验,确定了一致的同位素富集因子ε = -16.7/1000。使用100%铸铁和含28%铸铁/72%含水层基质混合物的柱实验也得到了-16.9/1000的富集因子。批次系统和柱系统之间富集因子的一致性表明,在批次系统中观察到的同位素趋势可能外推至诸如现场场地等流动系统。在所有实验中均观察到显著的同位素分馏这一事实意味着,同位素分析可以直接定性指示是否正在发生Fe0对TCE的还原脱氯。这一证据可能有助于回答现场场地出现的问题,例如确定在铁壁修复方案下游观察到的TCE是铁壁内降解不完全的结果,还是溶解的TCE羽流绕过铁壁的结果。