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Chlorine Isotope Fractionation of the Major Chloromethane Degradation Processes in the Environment.

Abstract

Chloromethane (CH3Cl) is an important source of chlorine in the stratosphere, but detailed knowledge of the magnitude of its sources and sinks is missing. Here, we measured the stable chlorine isotope fractionation (εCl) associated with the major abiotic and biotic CH3Cl sinks in the environment, namely, CH3Cl degradation by hydroxyl (·OH) and chlorine (·Cl) radicals in the troposphere and by reference bacteria Methylorubrum extorquens CM4 and Leisingera methylohalidivorans MB2 from terrestrial and marine environments, respectively. No chlorine isotope fractionation was detected for reaction of CH3Cl with ·OH and ·Cl radicals, whereas a large chlorine isotope fractionation (εCl) of -10.9 ± 0.7‰ (n = 3) and -9.4 ± 0.9 (n = 3) was found for CH3Cl degradation by M. extorquens CM4 and L. methylohalidivorans MB2, respectively. The large difference in chlorine isotope fractionation observed between tropospheric and bacterial degradation of CH3Cl provides an effective isotopic tool to characterize and distinguish between major abiotic and biotic processes contributing to the CH3Cl sink in the environment. Our findings demonstrate the potential of emerging triple-element isotopic approaches including chlorine to carbon and hydrogen analysis for the assessment of global cycling of organochlorines.

Authors+Show Affiliations

Institute of Earth Sciences , Heidelberg University , Im Neuenheimer Feld 236 , 69120 Heidelberg , Germany.Department of Geological Sciences , University of Texas , Austin , Texas 78712 , United States.Department of Isotope Biogeochemistry , Helmholtz Centre for Environmental Research - UFZ , Permoserstr.15 , 04318 Leipzig , Germany.Leibniz Institute for Baltic Sea Research Warnemünde , Seestrasse 15 , 18119 Rostock , Germany.UMR 7156 CNRS Génétique Moléculaire, Génomique, Microbiologie , Université de Strasbourg , 4 allée Konrad Roentgen , 67000 Strasbourg , France.UMR 7156 CNRS Génétique Moléculaire, Génomique, Microbiologie , Université de Strasbourg , 4 allée Konrad Roentgen , 67000 Strasbourg , France.Institute of Earth Sciences , Heidelberg University , Im Neuenheimer Feld 236 , 69120 Heidelberg , Germany.Institute of Earth Sciences , Heidelberg University , Im Neuenheimer Feld 236 , 69120 Heidelberg , Germany. Max Planck Institute for Chemistry , Hahn-Meitner-Weg 1 , 55128 Mainz , Germany.UMR 7156 CNRS Génétique Moléculaire, Génomique, Microbiologie , Université de Strasbourg , 4 allée Konrad Roentgen , 67000 Strasbourg , France.

Pub Type(s)

Journal Article

Language

eng

PubMed ID

31880153

Citation

Keppler, Frank, et al. "Chlorine Isotope Fractionation of the Major Chloromethane Degradation Processes in the Environment." Environmental Science & Technology, 2020.
Keppler F, Barnes JD, Horst A, et al. Chlorine Isotope Fractionation of the Major Chloromethane Degradation Processes in the Environment. Environ Sci Technol. 2020.
Keppler, F., Barnes, J. D., Horst, A., Bahlmann, E., Luo, J., Nadalig, T., ... Vuilleumier, S. (2020). Chlorine Isotope Fractionation of the Major Chloromethane Degradation Processes in the Environment. Environmental Science & Technology, doi:10.1021/acs.est.9b06139.
Keppler F, et al. Chlorine Isotope Fractionation of the Major Chloromethane Degradation Processes in the Environment. Environ Sci Technol. 2020 Jan 17; PubMed PMID: 31880153.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Chlorine Isotope Fractionation of the Major Chloromethane Degradation Processes in the Environment. AU - Keppler,Frank, AU - Barnes,Jaime D, AU - Horst,Axel, AU - Bahlmann,Enno, AU - Luo,Jing, AU - Nadalig,Thierry, AU - Greule,Markus, AU - Hartmann,S Christoph, AU - Vuilleumier,Stéphane, Y1 - 2020/01/17/ PY - 2019/12/28/pubmed PY - 2019/12/28/medline PY - 2019/12/28/entrez JF - Environmental science & technology JO - Environ. Sci. Technol. N2 - Chloromethane (CH3Cl) is an important source of chlorine in the stratosphere, but detailed knowledge of the magnitude of its sources and sinks is missing. Here, we measured the stable chlorine isotope fractionation (εCl) associated with the major abiotic and biotic CH3Cl sinks in the environment, namely, CH3Cl degradation by hydroxyl (·OH) and chlorine (·Cl) radicals in the troposphere and by reference bacteria Methylorubrum extorquens CM4 and Leisingera methylohalidivorans MB2 from terrestrial and marine environments, respectively. No chlorine isotope fractionation was detected for reaction of CH3Cl with ·OH and ·Cl radicals, whereas a large chlorine isotope fractionation (εCl) of -10.9 ± 0.7‰ (n = 3) and -9.4 ± 0.9 (n = 3) was found for CH3Cl degradation by M. extorquens CM4 and L. methylohalidivorans MB2, respectively. The large difference in chlorine isotope fractionation observed between tropospheric and bacterial degradation of CH3Cl provides an effective isotopic tool to characterize and distinguish between major abiotic and biotic processes contributing to the CH3Cl sink in the environment. Our findings demonstrate the potential of emerging triple-element isotopic approaches including chlorine to carbon and hydrogen analysis for the assessment of global cycling of organochlorines. SN - 1520-5851 UR - https://www.unboundmedicine.com/medline/citation/31880153/Chlorine_Isotope_Fractionation_of_the_Major_Chloromethane_Degradation_Processes_in_the_Environment_ L2 - https://dx.doi.org/10.1021/acs.est.9b06139 DB - PRIME DP - Unbound Medicine ER -