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2014-07-10

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Si us plau utilitzeu sempre aquest identificador per citar o enllaçar aquest document: https://hdl.handle.net/2445/163696

C and Cl isotope fractionation of 1,2-dichloroethane displays unique δ13C/δ37Cl patterns for pathway identification and reveals surprising C−Cl bond involvement in microbial oxidation

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https://doi.org/10.1021/es5031917

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This study investigated dual element isotope fractionation during aerobic biodegradation of 1,2-dichloroethane (1,2-DCA) via oxidative cleavage of a C-H bond (Pseudomonas sp. Strain DCA1) versus C-Cl bond cleavage by SN2 reaction (Xanthobacter autrophicus GJ10 and Ancylobacter aquaticus AD20). Compound-specific chlorine isotope analysis of 1,2-DCA was performed for the first time and isotope fractionation ε_bulk^Cl was determined by measurements of the same samples in three different laboratories using two GC-IRMS and one GC-quadrupole MS. Strongly pathway-dependent slopes (Δδ13C / Δδ37Cl), 0.78±0.03 (Oxidation) and 7.7±0.2 (SN2), delineate the potential of the dual isotope approach to identify 1,2-DCA degradation pathways in the field. In contrast to different ε_bulk^C values: -3.5±0.1¿ (Oxidation), -31.9±0.7¿ and -32.0±0.9¿ (SN2), the obtained ε_bulk^Cl values were surprisingly similar for the two pathways: -3.8±0.2¿ (Oxidation), -4.2±0.1¿ and -4.4±0.2¿ (SN2). Apparent kinetic isotope effects of 13C-AKIE=1.0070±0.0002 (Oxidation), 13C-AKIE=1.068±0.001 (SN2) and 37Cl-AKIE=1.0087±0.0002 (SN2) fell within expected ranges. In contrast, an unexpectedly large secondary 37Cl-AKIE of 1.0038±0.0002 reveal a hitherto unrecognized involvement of C-Cl bonds in microbial C-H bond oxidation. Our 2D isotope fractionation patterns enable for the first time reliable 1,2-DCA degradation pathway identification in the field, which unlocks the full potential of isotope applications for this important groundwater contaminant.

Matèries

Degradació ambiental, Clor, Isòtops de carboni

Matèries (anglès)

Environmental degradation, Chlorine, Carbon isotopes

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Articles publicats en revistes (Mineralogia, Petrologia i Geologia Aplicada)

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AUTOR PALAU, Jordi, et al. C and Cl isotope fractionation of 1,2-dichloroethane displays unique δ13C/δ37Cl patterns for pathway identification and reveals surprising C−Cl bond involvement in microbial oxidation. Environmental Science & Technology. 2014. Vol. 48, num. 16, pags. 9430-9437. ISSN 0013-936X. [consulted: 19 of August of 2026]. Available at: https://hdl.handle.net/2445/163696

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