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  • 1
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    Online Resource
    Carbon and Hydrogen Isotope Signatures of Dissolved Methane in the Scheldt Estuary
    Springer Science and Business Media LLC ; 2021
    In:  Estuaries and Coasts Vol. 44, No. 1 ( 2021-01), p. 137-146
    Details
    In: Estuaries and Coasts, Springer Science and Business Media LLC, Vol. 44, No. 1 ( 2021-01), p. 137-146
    Abstract: We collected water samples from the Scheldt estuary during December 2015 and November 2016 for methane (CH 4 ) concentration and isotopic composition (δ 13 C and δD values) analyses, to investigate the origin of the excess dissolved CH 4 , which is a common feature in estuaries. The Scheldt estuary is a eutrophic, heterotrophic tidal estuary, located at the border between Belgium and the Netherlands. The gas chromatography and mass spectrometry analyses revealed (1) variable dissolved CH 4 concentrations reaching up to 302.6 nM in surface waters of the Port of Antwerp, which fits within the higher range of values reported for European estuaries, and (2) the presence of surprisingly high isotopic signatures in the upper estuary. While microbial CH 4 production dominates in the lower part of the estuary, we observe a clear trend towards isotopically heavier CH 4 upstream where isotopic signatures as enriched as − 25.2‰ for carbon and + 101‰ for hydrogen were measured. We conclude that microbial oxidation of most of the CH 4 pool could explain such enrichments, but that the origin of riverine CH 4 enriched isotopic signatures remains to be explained. This study identifies peculiar features associated with CH 4 cycling in the Scheldt estuary, paving the way for a more thorough biogeochemical quantification of various production/removal processes.
    Type of Medium: Online Resource
    ISSN: 1559-2723 , 1559-2731
    URL: Article
    DOI: 10.1007/s12237-020-00768-3
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2021
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  • 2
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    Development and evaluation of a suite of isotope reference gases for methane in air
    Copernicus GmbH ; 2016
    In:  Atmospheric Measurement Techniques Vol. 9, No. 8 ( 2016-08-12), p. 3717-3737
    Details
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 9, No. 8 ( 2016-08-12), p. 3717-3737
    Abstract: Abstract. Measurements from multiple laboratories have to be related to unifying and traceable reference material in order to be comparable. However, such fundamental reference materials are not available for isotope ratios in atmospheric methane, which led to misinterpretations of combined data sets in the past. We developed a method to produce a suite of synthetic CH4-in-air standard gases that can be used to unify methane isotope ratio measurements of laboratories in the atmospheric monitoring community. Therefore, we calibrated a suite of pure methane gases of different methanogenic origin against international referencing materials that define the VSMOW (Vienna Standard Mean Ocean Water) and VPDB (Vienna Pee Dee Belemnite) isotope scales. The isotope ratios of our pure methane gases range between −320 and +40 ‰ for δ2H–CH4 and between −70 and −40 ‰ for δ13C–CH4, enveloping the isotope ratios of tropospheric methane (about −85 and −47 ‰ for δ2H–CH4 and δ13C–CH4 respectively). Estimated uncertainties, including the full traceability chain, are 〈 1.5 ‰ and 〈 0.2 ‰ for δ2H and δ13C calibrations respectively. Aliquots of the calibrated pure methane gases have been diluted with methane-free air to atmospheric methane levels and filled into 5 L glass flasks. The synthetic CH4-in-air standards comprise atmospheric oxygen/nitrogen ratios as well as argon, krypton and nitrous oxide mole fractions to prevent gas-specific measurement artefacts. The resulting synthetic CH4-in-air standards are referred to as JRAS-M16 (Jena Reference Air Set – Methane 2016) and will be available to the atmospheric monitoring community. JRAS-M16 may be used as unifying isotope scale anchor for isotope ratio measurements in atmospheric methane, so that data sets can be merged into a consistent global data frame.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    URL: Article
    URL: Article
    DOI: 10.5194/amt-9-3717-2016
    DOI: 10.5194/amt-9-3717-2016-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
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  • 3
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    Methane airborne measurements and comparison to global models during BARCA : METHANE IN THE AMAZON DURING BARCA
    American Geophysical Union (AGU) ; 2012
    In:  Journal of Geophysical Research: Atmospheres Vol. 117, No. D15 ( 2012-08-16), p. n/a-n/a
    Details
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 117, No. D15 ( 2012-08-16), p. n/a-n/a
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/2011JD017345
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2012
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  • 4
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    Interlaboratory comparison of 〈i〉δ〈/i〉〈sup〉13〈/sup〉C and 〈i〉δ〈/i〉D measurements of atmospheric CH〈sub〉4〈/sub〉 for combined use of data sets from different laboratories
    Copernicus GmbH ; 2018
    In:  Atmospheric Measurement Techniques Vol. 11, No. 2 ( 2018-03-02), p. 1207-1231
    Details
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 11, No. 2 ( 2018-03-02), p. 1207-1231
    Abstract: Abstract. We report results from a worldwide interlaboratory comparison of samples among laboratories that measure (or measured) stable carbon and hydrogen isotope ratios of atmospheric CH4 (δ13C-CH4 and δD-CH4). The offsets among the laboratories are larger than the measurement reproducibility of individual laboratories. To disentangle plausible measurement offsets, we evaluated and critically assessed a large number of intercomparison results, some of which have been documented previously in the literature. The results indicate significant offsets of δ13C-CH4 and δD-CH4 measurements among data sets reported from different laboratories; the differences among laboratories at modern atmospheric CH4 level spread over ranges of 0.5 ‰ for δ13C-CH4 and 13 ‰ for δD-CH4. The intercomparison results summarized in this study may be of help in future attempts to harmonize δ13C-CH4 and δD-CH4 data sets from different laboratories in order to jointly incorporate them into modelling studies. However, establishing a merged data set, which includes δ13C-CH4 and δD-CH4 data from multiple laboratories with desirable compatibility, is still challenging due to differences among laboratories in instrument settings, correction methods, traceability to reference materials and long-term data management. Further efforts are needed to identify causes of the interlaboratory measurement offsets and to decrease those to move towards the best use of available δ13C-CH4 and δD-CH4 data sets.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    URL: Article
    DOI: 10.5194/amt-11-1207-2018
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
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  • 5
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    Sources and sinks of methane in sea ice
    University of California Press ; 2021
    In:  Elementa: Science of the Anthropocene Vol. 9, No. 1 ( 2021-10-27)
    Details
    In: Elementa: Science of the Anthropocene, University of California Press, Vol. 9, No. 1 ( 2021-10-27)
    Abstract: We report on methane (CH4) stable isotope (δ13C and δ2H) measurements from landfast sea ice collected near Barrow (Utqiagvik, Alaska) and Cape Evans (Antarctica) over the winter-to-spring transition. These measurements provide novel insights into pathways of CH4 production and consumption in sea ice. We found substantial differences between the two sites. Sea ice overlying the shallow shelf of Barrow was supersaturated in CH4 with a clear microbial origin, most likely from methanogenesis in the sediments. We estimated that in situ CH4 oxidation consumed a substantial fraction of the CH4 being supplied to the sea ice, partly explaining the large range of isotopic values observed (δ13C between –68.5 and –48.5 ‰ and δ2H between –246 and –104 ‰). Sea ice at Cape Evans was also supersaturated in CH4 but with surprisingly high δ13C values (between –46.9 and –13.0 ‰), whereas δ2H values (between –313 and –113 ‰) were in the range of those observed at Barrow. These are the first measurements of CH4 isotopic composition in Antarctic sea ice. Our data set suggests a potential combination of a hydrothermal source, in the vicinity of the Mount Erebus, with aerobic CH4 formation in sea ice, although the metabolic pathway for the latter still needs to be elucidated. Our observations show that sea ice needs to be considered as an active biogeochemical interface, contributing to CH4 production and consumption, which disputes the standing paradigm that sea ice is an inert barrier passively accumulating CH4 at the ocean-atmosphere boundary.
    Type of Medium: Online Resource
    ISSN: 2325-1026
    URL: Article
    DOI: 10.1525/elementa.2020.00167
    Language: English
    Publisher: University of California Press
    Publication Date: 2021
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  • 6
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    High potential for CH 4 emission mitigation from oil infrastructure in one of EU's major production regions
    Copernicus GmbH ; 2023
    In:  Atmospheric Chemistry and Physics Vol. 23, No. 18 ( 2023-09-20), p. 10399-10412
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 18 ( 2023-09-20), p. 10399-10412
    Abstract: Abstract. Ambitious methane (CH4) emission mitigation represents one of the most effective opportunities to slow the rate of global warming over the next decades. The oil and gas (O&G) sector is a significant source of methane emissions, with technically feasible and cost-effective emission mitigation options. Romania, a key O&G producer within the EU, with the second highest reported annual CH4 emissions from the energy sector in the year 2020 (Greenhouse Gas Inventory Data - Comparison by Category, 2022), can play an important role towards the EU's emission reduction targets. In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. Measured emissions were characterized by heavily skewed distributions, with 10 % of the sites accounting for more than 70 % of total emissions. Integrating the results from all site-level quantifications with different approaches, we derive a central estimate of 5.4 kg h−1 per site of CH4 (3.6 %–8.4 %, 95 % confidence interval) for oil production sites. This estimate represents the third highest when compared to measurement-based estimates of similar facilities from other production regions. Based on our results, we estimate a total of 120 kt CH4 yr−1 (range: 79–180 kt yr−1) from oil production sites in our studied areas in Romania. This is approximately 2.5 times higher than the reported emissions from the entire Romanian oil production sector for 2020. Based on the source-level characterization, up to three-quarters of the detected emissions from oil production sites are related to operational venting. Our results suggest that O&G production infrastructure in Romania holds a massive mitigation potential, specifically by implementing measures to capture the gas and minimize operational venting and leaks.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    URL: Article
    DOI: 10.5194/acp-23-10399-2023
    DOI: 10.5194/acp-23-10399-2023-supplement
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
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  • 7
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    Atmospheric composition in the European Arctic and 30 years of the Zeppelin Observatory, Ny-Ålesund
    Copernicus GmbH ; 2022
    In:  Atmospheric Chemistry and Physics Vol. 22, No. 5 ( 2022-03-14), p. 3321-3369
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 5 ( 2022-03-14), p. 3321-3369
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-22-3321-2022
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 8
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    New contributions of measurements in Europe to the global inventory of the stable isotopic composition of methane
    Copernicus GmbH ; 2022
    In:  Earth System Science Data Vol. 14, No. 9 ( 2022-09-23), p. 4365-4386
    Details
    In: Earth System Science Data, Copernicus GmbH, Vol. 14, No. 9 ( 2022-09-23), p. 4365-4386
    Abstract: 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 https://doi.org/10.24416/UU01-YP43IN (Menoud et al., 2022a).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    URL: Article
    DOI: 10.5194/essd-14-4365-2022
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
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  • 9
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    Quantification of methane emissions in Hamburg using a network of FTIR spectrometers and an inverse modeling approach
    Copernicus GmbH ; 2023
    In:  Atmospheric Chemistry and Physics Vol. 23, No. 12 ( 2023-06-22), p. 6897-6922
    Details
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 12 ( 2023-06-22), p. 6897-6922
    Abstract: Abstract. Methane (CH4) is a potent greenhouse gas, and anthropogenic CH4 emissions contribute significantly to global warming. In this study, the CH4 emissions of the second most populated city in Germany, Hamburg, were quantified with measurements from four solar-viewing Fourier transform infrared (FTIR) spectrometers, mobile in situ measurements, and an inversion framework. For source type attribution, an isotope ratio mass spectrometer was deployed in the city. The urban district hosts an extensive industrial and port area in the south as well as a large conglomerate of residential areas north of the Elbe River. For emission modeling, the TNO GHGco (Netherlands Organisation for Applied Scientific Research greenhouse gas and co-emitted species emission database) inventory was used as a prior for the inversion. In order to improve the inventory, two approaches were followed: (1) the addition of a large natural CH4 source, the Elbe River, which was previously not included in the inventory, and (2) mobile measurements were carried out to update the spatial distribution of emissions in the TNO GHGco gridded inventory and derive two updated versions of the inventory. The addition of the river emissions improved model performance, whereas the correction of the spatial distribution with mobile measurements did not have a significant effect on the total emission estimates for the campaign period. A comparison of the updated inventories with emission estimates from a Gaussian plume model (GPM) showed that the updated versions of the inventory match the GPM emissions estimates well in several cases, revealing the potential of mobile measurements to update the spatial distribution of emission inventories. The mobile measurement survey also revealed a large and, at the time of the study, unknown point source of thermogenic origin with a magnitude of 7.9 ± 5.3 kg h−1 located in a refinery. The isotopic measurements show strong indications that there is a large biogenic CH4 source in Hamburg that produced repeated enhancements of over 1 ppm which correlated with the rising tide of the river estuary. The CH4 emissions (anthropogenic and natural) of the city of Hamburg were quantified as 1600 ± 920 kg h−1, 900 ± 510 kg h−1 of which is of anthropogenic origin. This study reveals that mobile street-level measurements may miss the majority of total methane emissions, potentially due to sources located within buildings, including stoves and boilers operating on natural gas. Similarly, the CH4 enhancements recorded during the mobile survey from large-area sources, such as the Alster lakes, were too small to generate GPM emission estimates with confidence, but they could nevertheless influence the emission estimates based on total column measurements.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    URL: Article
    DOI: 10.5194/acp-23-6897-2023
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
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  • 10
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    Isotopic composition of H 2 from wood burning: Dependency on combustion efficiency, moisture content, and δ D of local precipitation
    American Geophysical Union (AGU) ; 2010
    In:  Journal of Geophysical Research Vol. 115, No. D17 ( 2010-09-15)
    Details
    In: Journal of Geophysical Research, American Geophysical Union (AGU), Vol. 115, No. D17 ( 2010-09-15)
    Type of Medium: Online Resource
    ISSN: 0148-0227
    URL: Article
    DOI: 10.1029/2009JD013188
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2010
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