| 1. |
- Jansen, Joachim, et al.
(författare)
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The origin of methane in the East Siberian Arctic Shelf unraveled with triple isotope analysis
- 2017
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Ingår i: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 14:9, s. 2283-2292
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Tidskriftsartikel (refereegranskat)abstract
- The Arctic Ocean, especially the East Siberian Arctic Shelf (ESAS), has been proposed as a significant source of methane that might play an increasingly important role in the future. However, the underlying processes of formation, removal and transport associated with such emissions are to date strongly debated. CH4 concentration and triple isotope composition were analyzed on gas extracted from sediment and water sampled at numerous locations on the shallow ESAS from 2007 to 2013. We find high concentrations (up to 500 µM) of CH4 in the pore water of the partially thawed subsea permafrost of this region. For all sediment cores, both hydrogen and carbon isotope data reveal the predominant occurrence of CH4 that is not of thermogenic origin as it has long been thought, but resultant from microbial CH4 formation. At some locations, meltwater from buried meteoric ice and/or old organic matter preserved in the subsea permafrost were used as sub-strates. Radiocarbon data demonstrate that the CH4 present in the ESAS sediment is of Pleistocene age or older, but a small contribution of highly C-14-enriched CH4, from unknown origin, prohibits precise age determination for one sediment core and in the water column. Our sediment data suggest that at locations where bubble plumes have been observed, CH4 can escape anaerobic oxidation in the surface sediment.
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| 2. |
- Menoud, Malika, et al.
(författare)
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New contributions of measurements in Europe to the global inventory of the stable isotopic composition of methane
- 2022
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Ingår i: Earth System Science Data. - : Copernicus GmbH. - 1866-3508 .- 1866-3516. ; 14:9, s. 4365-4386
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Tidskriftsartikel (refereegranskat)abstract
- Recent climate change mitigation strategies rely on the reduction of methane (CH4) emissions. Carbon and hydrogen isotope ratio (δ13CCH4 and δ2HCH4) measurements can be used to distinguish sources and thus to understand the CH4 budget better. The CH4 emission estimates by models are sensitive to the isotopic signatures assigned to each source category, so it is important to provide representative estimates of the different CH4 source isotopic signatures worldwide. We present new measurements of isotope signatures of various, mainly anthropogenic, CH4 sources in Europe, which represent a substantial contribution to the global dataset of source isotopic measurements from the literature, especially for δ2HCH4. They improve the definition of δ13CCH4 from waste sources, and demonstrate the use of δ2HCH4 for fossil fuel source attribution. We combined our new measurements with the last published database of CH4 isotopic signatures and with additional literature, and present a new global database. We found that microbial sources are generally well characterised. The large variability in fossil fuel isotopic compositions requires particular care in the choice of weighting criteria for the calculation of a representative global value. The global dataset could be further improved by measurements from African, South American, and Asian countries, and more measurements from pyrogenic sources. We improved the source characterisation of CH4 emissions using stable isotopes and associated uncertainty, to be used in top-down studies. We emphasise that an appropriate use of the database requires the analysis of specific parameters in relation to source type and the region of interest. The final version of the European CH4 isotope database coupled with a global inventory of fossil and non-fossil δ13CCH4 and δ2HCH4 source signature measurements is available at 10.24416/UU01-YP43IN .
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| 3. |
- Platt, Stephen M., et al.
(författare)
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Atmospheric composition in the European Arctic and 30 years of the Zeppelin Observatory, Ny-Ålesund
- 2022
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:5, s. 3321-3369
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Tidskriftsartikel (refereegranskat)abstract
- The Zeppelin Observatory (78.90∘ N, 11.88∘ E) is located on Zeppelin Mountain at 472 m a.s.l. on Spitsbergen, the largest island of the Svalbard archipelago. Established in 1989, the observatory is part of Ny-Ålesund Research Station and an important atmospheric measurement site, one of only a few in the high Arctic, and a part of several European and global monitoring programmes and research infrastructures, notably the European Monitoring and Evaluation Programme (EMEP); the Arctic Monitoring and Assessment Programme (AMAP); the Global Atmosphere Watch (GAW); the Aerosol, Clouds and Trace Gases Research Infrastructure (ACTRIS); the Advanced Global Atmospheric Gases Experiment (AGAGE) network; and the Integrated Carbon Observation System (ICOS). The observatory is jointly operated by the Norwegian Polar Institute (NPI), Stockholm University, and the Norwegian Institute for Air Research (NILU). Here we detail the establishment of the Zeppelin Observatory including historical measurements of atmospheric composition in the European Arctic leading to its construction. We present a history of the measurements at the observatory and review the current state of the European Arctic atmosphere, including results from trends in greenhouse gases, chlorofluorocarbons (CFCs) and hydrochlorofluorocarbons (HCFCs), other traces gases, persistent organic pollutants (POPs) and heavy metals, aerosols and Arctic haze, and atmospheric transport phenomena, and provide an outline of future research directions.
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| 4. |
- Röckmann, Thomas, et al.
(författare)
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In situ observations of the isotopic composition of methane at the Cabauw tall tower site
- 2016
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:16, s. 10469-10487
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Tidskriftsartikel (refereegranskat)abstract
- High-precision analyses of the isotopic composition of methane in ambient air can potentially be used to discriminate between different source categories. Due to the complexity of isotope ratio measurements, such analyses have generally been performed in the laboratory on air samples collected in the field. This poses a limitation on the temporal resolution at which the isotopic composition can be monitored with reasonable logistical effort. Here we present the performance of a dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique for in situ analysis of the isotopic composition of methane under field conditions. Both systems were deployed at the Cabauw Experimental Site for Atmospheric Research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months. The IRMS and QCLAS instruments were in excellent agreement with a slight systematic offset of (+0.25±0.04)‰ for δ13C and (-4.3±0.4)‰ for δD. This was corrected for, yielding a combined dataset with more than 2500 measurements of both δ13C and δD. The high-precision and hightemporal- resolution dataset not only reveals the overwhelming contribution of isotopically depleted agricultural CH4 emissions from ruminants at the Cabauw site but also allows the identification of specific events with elevated contributions from more enriched sources such as natural gas and landfills. The final dataset was compared to model calculations using the global model TM5 and the mesoscale model FLEXPART-COSMO. The results of both models agree better with the measurements when the TNO-MACC emission inventory is used in the models than when the EDGAR inventory is used. This suggests that high-resolution isotope measurements have the potential to further constrain the methane budget when they are performed at multiple sites that are representative for the entire European domain.
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