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Hydrocarbons to Carboxyl-Rich Alicyclic Molecules: A Continuum Model to Describe Biodegradation of Petroleum-Derived Dissolved Organic Matter in Contaminated Groundwater Plumes
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2020-09-19 , DOI: 10.1016/j.jhazmat.2020.123998
David C. Podgorski , Phoebe Zito , Anne M. Kellerman , Barbara A. Bekins , Isabelle M. Cozzarelli , Donald F. Smith , Xiaoyan Cao , Klaus Schmidt-Rohr , Sasha Wagner , Aron Stubbins , Robert G.M. Spencer

Relationships between dissolved organic matter (DOM) reactivity and chemical composition in a groundwater plume containing petroleum-derived DOM were examined by quantitative and qualitative measurements to determine the source and chemical composition of the compounds that persist downgradient. Samples were collected from a transect down the core of the plume in the direction of groundwater flow. An exponential decrease in dissolved organic carbon concentration resulting from biodegradation along the transect correlated with a continuous shift in fluorescent DOM from shorter to longer wavelengths. Moreover, ultrahigh resolution mass spectrometry showed a shift from low molecular weight (MW) aliphatic, reduced compounds to high MW, unsaturated (alicyclic/aromatic), high oxygen compounds that are consistent with carboxyl-rich alicyclic molecules. The degree of condensed aromaticity increased downgradient, indicating that compounds with larger, conjugated aromatic core structures were less susceptible to biodegradation. Nuclear magnetic resonance spectroscopy showed a decrease in alkyl (particularly methyl) and an increase in aromatic/olefinic structural motifs. Collectively, data obtained from the combination of these complementary analytical techniques indicated that changes in the DOM composition of a groundwater plume are gradual, as relatively low molecular weight (MW), reduced, aliphatic compounds from the oil source were selectively degraded and high MW, alicyclic/aromatic, oxidized compounds persisted.



中文翻译:

碳氢化合物转化为富含羧基的脂环族分子:描述被石油污染的地下水羽中石油衍生的溶解有机物生物降解的连续模型

通过定量和定性测量来检查含有石油衍生的DOM的地下水羽中溶解有机物(DOM)反应性与化学组成之间的关系,以确定持续下降的化合物的来源和化学组成。沿地下水流的方向从羽状岩心下方的横断面收集样品。沿着横断面的生物降解导致的溶解有机碳浓度的指数下降与荧光DOM从较短波长到较长波长的连续移动相关。此外,超高分辨率质谱显示从低分子量(MW)的脂肪族还原化合物转变为与富含羧基的脂环族分子一致的高MW,不饱和(脂环族/芳族)高氧化合物。稠合芳族化合物的程度降低了梯度,表明具有较大共轭芳族核结构的化合物较不易被生物降解。核磁共振波谱显示烷基(特别是甲基)的减少和芳烃/烯烃结构基序的增加。总的来说,从这些互补的分析技术的组合中获得的数据表明,地下水羽流中DOM组成的变化是渐进的,因为相对较低的分子量(MW),还原的,来自油源的脂肪族化合物被选择性地降解,并且高MW,脂环族/芳族氧化化合物持续存在。核磁共振波谱显示烷基(特别是甲基)的减少和芳烃/烯烃结构基序的增加。总的来说,从这些互补的分析技术的组合中获得的数据表明,地下水羽流中DOM组成的变化是渐进的,因为相对较低的分子量(MW),还原的,来自油源的脂肪族化合物被选择性地降解,并且高MW,脂环族/芳族氧化化合物持续存在。核磁共振波谱显示烷基(特别是甲基)的减少和芳烃/烯烃结构基序的增加。总的来说,从这些互补的分析技术的组合中获得的数据表明,地下水羽流中DOM组成的变化是渐进的,因为相对较低的分子量(MW),还原的,来自油源的脂肪族化合物被选择性地降解,并且高MW,脂环族/芳族氧化化合物持续存在。

更新日期:2020-09-20
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