PuSH - Publication Server of Helmholtz Zentrum München: C and Cl isotope fractionation of 1,2-dichloroethane displays unique δ<sup>13</sup>C/δ<sup>37</sup>Cl patterns for pathway identification and reveals surprising C-Cl bond involvement in microbial oxidation.

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Palau, J.* ; Cretnik, S. ; Shouakar-Stash, O.* ; Höche, M. ; Elsner, M. ; Hunkeler, D.*

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.

Environ. Sci. Technol. 48, 9430-9437 (2014)

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This study investigates 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 S_N2 reaction (Xanthobacter autotrophicus 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 gas chromatography–isotope ratio mass spectrometry systems and one gas chromatography–quadrupole mass spectrometry system. Strongly pathway-dependent slopes (Δδ¹³C/Δδ³⁷Cl), 0.78 ± 0.03 (oxidation) and 7.7 ± 0.2 (S_N2), 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) and −31.9 ± 0.7 and −32.0 ± 0.9‰ (S_N2)], the obtained ε_bulk^Cl values were surprisingly similar for the two pathways: −3.8 ± 0.2‰ (oxidation) and −4.2 ± 0.1 and −4.4 ± 0.2‰ (S_N2). Apparent kinetic isotope effects (AKIEs) of 1.0070 ± 0.0002 (¹³C-AKIE, oxidation), 1.068 ± 0.001 (¹³C-AKIE, S_N2), and 1.0087 ± 0.0002 (³⁷Cl-AKIE, S_N2) fell within expected ranges. In contrast, an unexpectedly large secondary ³⁷Cl-AKIE of 1.0038 ± 0.0002 reveals a hitherto unrecognized involvement of C–Cl bonds in microbial C–H bond oxidation. Our two-dimensional isotope fractionation patterns allow 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.

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PuSH - Publication Server of Helmholtz Zentrum München

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.

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.