Abstract
Abstract. The carbon isotopic signature (δ13CH4) of several methane sources in Germany (around Heidelberg and in North Rhine-Westphalia) were characterised. Mobile measurements of the plume of CH4 sources are carried out using an analyser based on cavity ring-down spectroscopy (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 composition differences of the gas matrix in air samples or calibration tanks. The two most important gases which affect δ13CH4 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 typically abundant in natural gases 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 by up to 3 ‰ depending on whether a C2H6 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 signatures 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 November 2018 gas samples from the Heidelberg natural gas distribution network were measured with a mean δ13CH4 value of -43.3±0.8‰. Contrary to previous measurements between 1991 and 1996 by Levin et al. (1999), no strong seasonal cycle is shown.
Highlights
Methane (CH4) is the second most important anthropogenic greenhouse gas
The source categories can be classified as pyrogenic, biogenic or thermogenic, which show different and overlapping isotope ratio ranges
The average was −46.6 ± 6.8 ‰ and a little bit less enriched than the isotopic signatures of CH4 measured in Sandhausen and than the natural gas samples taken in Heidelberg (−43.3 ± 0.8 ‰)
Summary
Methane (CH4) is the second most important anthropogenic greenhouse gas. The atmospheric growth rate of CH4 has changed significantly during the last decades, stabilising at zero growth from 1999 to 2006 before beginning to increase again after 2007 (Dlugokencky et al, 2009). In addition to seasonal variations, changes in landfill managements like gas collector systems and the implementation of biogas plants at many farms need to be taken into account for a new study of the global and regional source signature of CH4. Instrumental development in measurement technique allows isotope analysis of δ13CH4 by a CRDS analyser and even its use on a mobile platform (Rella et al, 2015; Lopez et al, 2017). This is a further improvement to the study of Zazzeri et al (2015), which involved collecting air samples in bags and analysing them later in the laboratory by IRMS. During 21 mobile measurement days, emission plumes from a biogas plant, three dairy farms, a landfill, a wastewater treatment plant, two natural gas facilities and a bituminous deep coal mine were measured with our set-up
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