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Atmospheric Measurement Techniques An interactive open-access journal of the European Geosciences Union
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Discussion papers
https://doi.org/10.5194/amt-2018-259
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-2018-259
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 01 Oct 2018

Research article | 01 Oct 2018

Review status
This discussion paper is a preprint. A revision of the manuscript is under review for the journal Atmospheric Measurement Techniques (AMT).

Characterisation of δ13CH4 source signatures from methane sources in Germany using mobile measurements

Antje Hoheisel1, Christiane Yeman1,a, Florian Dinger1,2, Henrik Eckhardt1, and Martina Schmidt1 Antje Hoheisel et al.
  • 1Institute of Environmental Physics, Heidelberg University, Heidelberg, Germany
  • 2Max-Planck Institute for Chemistry, Mainz, Germany
  • anow at: Laboratory of Ion Beam Physics, ETH Zurich, Zurich, Switzerland

Abstract. The carbon isotopic signature (δ13CH4) of several methane sources in Germany (around Heidelberg and in North Rhine-Westphalia) were characterised. Therefore, mobile measurements of the plume of CH4 sources are carried out using a cavity ring-down spectrometer (CRDS). To achieve precise results a CRDS analyser, which measures methane (CH4), carbon dioxide (CO2) and their 13C to 12C ratios, was characterised especially with regard to cross sensitivities of the gas matrix. The two most important gases which affect the measurements are water vapour (H2O) and ethane (C2H6). To avoid the cross sensitivity with H2O, the air is dried with a nafion dryer during mobile measurements. C2H6 is abundant in natural gas and thus in methane plumes or samples originating from natural gas. A C2H6 correction and calibration are essential to obtain accurate δ13CH4 results, which can deviate up to 3‰ depending on whether an ethane correction is applied.

The isotopic signature is determined with the Miller-Tans approach and the York fitting method. During 21 field campaigns the mean δ13CH4 values of three dairy farms (−63.9±0.9‰), a biogas plant (−62.4±1.2‰), a landfill (−58.7±3.3‰), a wastewater treatment plant (−52.5±1.4‰), an active deep coal mine (−56.0±2.3‰) and two natural gas storage and gas compressor stations (−46.1±0.8‰) were recorded.

In addition, between December 2016 and June 2018 gas samples from the Heidelberg natural gas distribution network were measured. Contrary to former measurements between 1991 and 1996 (Levin et al., 1999) no strong seasonal cycle is shown. The mean δ13CH4 value of this study is −43.1±0.8‰ which is 2.8‰ more depleted than in former years.

Antje Hoheisel et al.
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Status: final response (author comments only)
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Antje Hoheisel et al.
Antje Hoheisel et al.
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Short summary
In this study, we developed and applied a mobile instrument setup to determine the δ13CH4 signature by measuring the plume of different CH4 sources using a CRDS analyser. Therefore, we carefully characterised the CRDS analyser especially with regard to cross sensitivities of the gas matrix. During 21 field campaigns we determined mean δ13CH4 values of three dairy farms, a biogas plant, a landfill, a wastewater treatment plant, an active deep coal mine and two natural gas facilities in Germany.
In this study, we developed and applied a mobile instrument setup to determine the δ13CH4...
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