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富含脱氯菌属的富集培养物中二氯乙烷脱氯消除过程中的双碳-氯同位素分馏作用

Dual carbon - chlorine isotope fractionation during dichloroelimination of 1,1,2-trichloroethane by an enrichment culture containing Dehalogenimonas sp.

机构信息

Grup MAiMA, Mineralogia Aplicada, Geoquímica i Geomicrobiologia, Departament de Mineralogia, Petrologia i Geologia Aplicada, Facultat de Ciències de la Terra, Universitat de Barcelona (UB), Martí Franquès s/n, 08028 Barcelona, Spain.

Grup MAiMA, Mineralogia Aplicada, Geoquímica i Geomicrobiologia, Departament de Mineralogia, Petrologia i Geologia Aplicada, Facultat de Ciències de la Terra, Universitat de Barcelona (UB), Martí Franquès s/n, 08028 Barcelona, Spain; Institute of Environmental Assessment and Water Research (IDAEA), CSIC, Hydrogeology Group (UPC-CSIC), Jordi Girona 18-26, 08034 Barcelona, Spain.

出版信息

Sci Total Environ. 2019 Jan 15;648:422-429. doi: 10.1016/j.scitotenv.2018.08.071. Epub 2018 Aug 6.

Abstract

Chlorinated ethanes are frequent groundwater contaminants but compound specific isotope analysis (CSIA) has been scarcely applied to investigate their degradation pathways. In this study, dual carbon and chlorine isotope fractionation was used to investigate for the first time the anoxic biodegradation of 1,1,2-trichloroethane (1,1,2-TCA) using a Dehalogenimonas-containing culture. The isotopic fractionation values obtained for the biodegradation of 1,1,2-TCA were ɛ = -6.9 ± 0.4‰ and ɛ = -2.7 ± 0.3‰. The detection of vinyl chloride (VC) as unique byproduct and a closed carbon isotopic mass balance corroborated that dichloroelimination was the degradation pathway used by this strain. Combining the values of δC and δCl resulted in a dual element C-Cl isotope slope of Λ = 2.5 ± 0.2‰. Investigation of the apparent kinetic isotope effects (AKIEs) expected for cleavage of a CCl bond showed an important masking of the intrinsic isotope fractionation. Theoretical calculation of Λ suggested that dichloroelimination of 1,1,2-TCA was taking place via simultaneous cleavage of two CCl bonds (concerted reaction mechanism). The isotope data obtained in this study can be useful to monitor natural attenuation of 1,1,2-TCA via dichloroelimination and provide insights into the source and fate of VC in contaminated groundwaters.

摘要

氯乙烷是常见的地下水污染物,但化合物特定同位素分析(CSIA)很少被用于研究其降解途径。在这项研究中,首次使用含有 Dehalogenimonas 的培养物,通过双碳和氯同位素分馏来研究 1,1,2-三氯乙烷(1,1,2-TCA)的缺氧生物降解。1,1,2-TCA 生物降解的同位素分馏值为ɛ = -6.9 ± 0.4‰和ɛ = -2.7 ± 0.3‰。作为唯一副产物的氯乙烯(VC)的检测和封闭的碳同位素质量平衡证实了双氯消除是该菌株使用的降解途径。结合 δC 和 δCl 的值得到了双元素 C-Cl 同位素斜率 Λ = 2.5 ± 0.2‰。对预期用于 CCl 键断裂的表观动力学同位素效应(AKIEs)的研究表明,内在同位素分馏被重要地掩盖了。Λ 的理论计算表明,1,1,2-TCA 的双氯消除是通过同时断裂两个 CCl 键(协同反应机制)发生的。本研究获得的同位素数据可用于监测通过双氯消除自然衰减 1,1,2-TCA,并深入了解受污染地下水中 VC 的来源和归宿。

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