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Carbon Isotope Fractionation during Anaerobic Degradation of Methyl tert-Butyl Ether under Sulfate-Reducing and Methanogenic Conditions

机译:硫酸盐还原和产甲烷条件下甲基叔丁基醚厌氧降解过程中的碳同位素分馏

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摘要

Methyl tert-butyl ether (MTBE), an octane enhancer and a fuel oxygenate in reformulated gasoline, has received increasing public attention after it was detected as a major contaminant of water resources. Although several techniques have been developed to remediate MTBE-contaminated sites, the fate of MTBE is mainly dependent upon natural degradation processes. Compound-specific stable isotope analysis has been proposed as a tool to distinguish the loss of MTBE due to biodegradation from other physical processes. Although MTBE is highly recalcitrant, anaerobic degradation has been demonstrated under different anoxic conditions and may be an important process. To accurately assess in situ MTBE degradation through carbon isotope analysis, carbon isotope fractionation during MTBE degradation by different cultures under different electron-accepting conditions needs to be investigated. In this study, carbon isotope fractionation during MTBE degradation under sulfate-reducing and methanogenic conditions was studied in anaerobic cultures enriched from two different sediments. Significant enrichment of 13C in residual MTBE during anaerobic biotransformation was observed under both sulfate-reducing and methanogenic conditions. The isotopic enrichment factors (ɛ) estimated for each enrichment were almost identical (−13.4 to −14.6; r2 = 0.89 to 0.99). A ɛ value of −14.4 ± 0.7 was obtained from regression analysis (r2 = 0.97, n = 55, 95% confidence interval), when all data from our MTBE-transforming anaerobic cultures were combined. The similar magnitude of carbon isotope fractionation in all enrichments regardless of culture or electron-accepting condition suggests that the terminal electron-accepting process may not significantly affect carbon isotope fractionation during anaerobic MTBE degradation.
机译:甲基叔丁基醚(MTBE),辛烷值增强剂和重新配制汽油中的燃料含氧化合物在被检测为水资源的主要污染物后,受到了越来越多的公众关注。尽管已开发出多种技术来补救受MTBE污染的部位,但MTBE的命运主要取决于自然降解过程。已经提出了化合物特异性的稳定同位素分析作为区分由于生物降解引起的MTBE损失与其他物理过程的工具。尽管MTBE具有高度的顽强性,但已证明在不同的缺氧条件下厌氧降解可能是重要的过程。为了通过碳同位素分析准确评估MTBE的原位降解,需要研究在不同电子接受条件下不同培养物在MTBE降解过程中的碳同位素分馏。在这项研究中,在富集两种不同沉积物的厌氧培养物中,研究了硫酸盐还原和产甲烷条件下MTBE降解过程中的碳同位素分馏。在硫酸盐还原和产甲烷条件下,厌氧生物转化过程中残留的MTBE中的 13 C明显富集。每次富集估算的同位素富集因子(ɛ)几乎相同(-13.4至-14.6; r 2 = 0.89至0.99)。当将来自我们转化MTBE的厌氧培养物的所有数据进行合并时,通过回归分析得出1值为-14.4±0.7(r 2 = 0.97,n = 55,置信区间为95%)。不论培养物或电子接受条件如何,所有浓缩物中碳同位素分馏的大小相似,这表明在厌氧MTBE降解过程中,末端电子接受过程可能不会显着影响碳同位素分馏。

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