Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures
<p>Anthropogenic emissions are the primary source of the increase in atmospheric methane (<span class="inline-formula">CH<sub>4</sub></span>) levels. However, estimates of anthropogenic <span class="inline-formula">CH<sub>4</sub><...
| Main Authors: | , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Copernicus Publications
2023-12-01
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| Series: | Atmospheric Chemistry and Physics |
| Online Access: | https://acp.copernicus.org/articles/23/15749/2023/acp-23-15749-2023.pdf |
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| author | A. Fiehn M. Eckl J. Kostinek M. Gałkowski M. Gałkowski C. Gerbig M. Rothe T. Röckmann M. Menoud M. Menoud H. Maazallahi M. Schmidt P. Korbeń J. Neçki M. Stanisavljević M. Stanisavljević J. Swolkień A. Fix A. Roiger |
| author_facet | A. Fiehn M. Eckl J. Kostinek M. Gałkowski M. Gałkowski C. Gerbig M. Rothe T. Röckmann M. Menoud M. Menoud H. Maazallahi M. Schmidt P. Korbeń J. Neçki M. Stanisavljević M. Stanisavljević J. Swolkień A. Fix A. Roiger |
| author_sort | A. Fiehn |
| collection | DOAJ |
| description | <p>Anthropogenic emissions are the primary source of the increase in atmospheric methane (<span class="inline-formula">CH<sub>4</sub></span>) levels. However, estimates of anthropogenic <span class="inline-formula">CH<sub>4</sub></span> emissions still show large uncertainties at global and regional scales. Differences in <span class="inline-formula">CH<sub>4</sub></span> isotopic source signatures <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> can help to constrain different source contributions (e.g., fossil, waste, agriculture). The Upper Silesian Coal Basin (USCB) represents one of the largest European <span class="inline-formula">CH<sub>4</sub></span> emission regions, with more than 500 <span class="inline-formula">Gg CH<sub>4</sub> yr<sup>−1</sup></span> released from more than 50 coal mine ventilation shafts, landfills, and wastewater treatment plants. During the CoMet (Carbon Dioxide and Methane Mission) campaign in June 2018 methane observations were conducted from a variety of platforms including aircraft and cars to quantify these emissions. Besides the continuous sampling of atmospheric methane concentration, numerous air samples were taken from inside and around the ventilation shafts (1–2 km distance) and aboard the <i>High Altitude and Long Range Research Aircraft</i> (<i>HALO</i>) and DLR Cessna Caravan aircraft, and they were analyzed in the laboratory for the isotopic composition of <span class="inline-formula">CH<sub>4</sub></span>.</p>
<p>The airborne samples downwind of the USCB contained methane from the entire region and thus enabled determining the mean signature of the USCB accurately. This mean isotopic signature of methane emissions was <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M9" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">50.9</mn><mo>±</mo><mn mathvariant="normal">0.7</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="58pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="a27e853300f83c7b4b62be35f9825060"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00001.svg" width="58pt" height="10pt" src="acp-23-15749-2023-ie00001.png"/></svg:svg></span></span> ‰ for <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M11" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">226</mn><mo>±</mo><mn mathvariant="normal">9</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="46pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="4896105601a81a208b2037917e9548d2"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00002.svg" width="46pt" height="10pt" src="acp-23-15749-2023-ie00002.png"/></svg:svg></span></span> ‰ for <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>. This is in the range of previous USCB studies based on samples taken within the mines for <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> but more depleted in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> than reported before. Signatures of methane enhancements sampled upwind of the mines and in the free troposphere clearly showed the influence of biogenic sources. We determined the source signatures of individual coal mine ventilation shafts using ground-based samples. These signatures displayed a considerable range between different mines and also varied for individual shafts from day to day. Different layers of the USCB coal contain thermogenic methane, isotopically similar to natural gas, and methane formed through biogenic carbonate reduction. The signatures vary depending on what layer of coal is mined at the time of sampling. Mean shaft signatures range from <span class="inline-formula">−</span>60 ‰ to <span class="inline-formula">−</span>42 ‰ for <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and from <span class="inline-formula">−</span>200 ‰ to <span class="inline-formula">−</span>160 ‰ for <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>. A gradient in the signatures of subregions of the USCB is reflected both in the aircraft data and in the ground samples, with emissions from the southwest being most depleted in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> and emissions from the south being most depleted in <span class="inline-formula"><i>δ</i><sup>13</sup>C</span>, which is probably associated with the structural<span id="page15750"/> and lithostratigraphic history of the USCB and generation and migration processes of methane in the coal. The average signature of <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M23" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">49.8</mn><mo>±</mo><mn mathvariant="normal">5.7</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="58pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="c758e6ea1b22e7cd63c215ef195ab0da"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00003.svg" width="58pt" height="10pt" src="acp-23-15749-2023-ie00003.png"/></svg:svg></span></span> ‰ in <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M25" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">184</mn><mo>±</mo><mn mathvariant="normal">32</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="52pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="3b4d5869550ea9083ee077728cf29fbd"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00004.svg" width="52pt" height="10pt" src="acp-23-15749-2023-ie00004.png"/></svg:svg></span></span> ‰ in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> from the ventilation shafts clearly differs from the USCB regional signature in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>. This makes a source attribution using <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> signatures possible, which would not be possible with only the <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> isotopic signatures. We assume that the USCB plume mainly contains fossil coal mine methane and biogenic methane from waste treatment, because the USCB is a highly industrialized region with few other possible methane sources. Assuming a biogenic methane signature between and <span class="inline-formula">−</span>320 ‰ and <span class="inline-formula">−</span>280 ‰ for <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>, the biogenic methane emissions from the USCB account for 15 %–50 % of total emissions. The uncertainty range shows the need of comprehensive and extensive sampling from all possible source sectors for source apportionment. The share of anthropogenic–biogenic emissions of 0.4 %–14 % from this densely populated industrial region is underestimated in commonly used emission inventories. Generally, this study demonstrates the importance of <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>-<span class="inline-formula">CH<sub>4</sub></span> observations for methane source apportionment in regions with a mix of thermogenic and biogenic sources and, especially in our case, where the <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> signature of the coal mine gas has a large variability.</p> |
| first_indexed | 2024-03-08T21:18:24Z |
| format | Article |
| id | doaj.art-6e14cc407ede4ebd94d6f519c3d874ac |
| institution | Directory Open Access Journal |
| issn | 1680-7316 1680-7324 |
| language | English |
| last_indexed | 2024-03-08T21:18:24Z |
| publishDate | 2023-12-01 |
| publisher | Copernicus Publications |
| record_format | Article |
| series | Atmospheric Chemistry and Physics |
| spelling | doaj.art-6e14cc407ede4ebd94d6f519c3d874ac2023-12-21T12:54:08ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242023-12-0123157491576510.5194/acp-23-15749-2023Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signaturesA. Fiehn0M. Eckl1J. Kostinek2M. Gałkowski3M. Gałkowski4C. Gerbig5M. Rothe6T. Röckmann7M. Menoud8M. Menoud9H. Maazallahi10M. Schmidt11P. Korbeń12J. Neçki13M. Stanisavljević14M. Stanisavljević15J. Swolkień16A. Fix17A. Roiger18Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, GermanyDeutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, GermanyDeutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, GermanyMax Planck Institute for Biogeochemistry (MPI-BGC), Department of Biogeochemical Signals, Jena, GermanyFaculty of Physics and Applied Computer Science, AGH University of Kraków, Kraków, PolandMax Planck Institute for Biogeochemistry (MPI-BGC), Department of Biogeochemical Signals, Jena, GermanyMax Planck Institute for Biogeochemistry (MPI-BGC), Department of Biogeochemical Signals, Jena, GermanyInstitute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, the NetherlandsInstitute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, the NetherlandsLaboratoire des Sciences du Climat et de l'Environnement, Université de Versailles Saint-Quentin, Paris, FranceInstitute for Marine and Atmospheric research Utrecht (IMAU), Utrecht University, Utrecht, the NetherlandsInstitute of Environmental Physics, Heidelberg University, Heidelberg, GermanyInstitute of Environmental Physics, Heidelberg University, Heidelberg, GermanyFaculty of Physics and Applied Computer Science, AGH University of Kraków, Kraków, PolandFaculty of Physics and Applied Computer Science, AGH University of Kraków, Kraków, PolandFaculty of Civil Engineering and Resource Management, AGH University of Kraków, Kraków, PolandFaculty of Civil Engineering and Resource Management, AGH University of Kraków, Kraków, PolandDeutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, GermanyDeutsches Zentrum für Luft- und Raumfahrt (DLR), Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany<p>Anthropogenic emissions are the primary source of the increase in atmospheric methane (<span class="inline-formula">CH<sub>4</sub></span>) levels. However, estimates of anthropogenic <span class="inline-formula">CH<sub>4</sub></span> emissions still show large uncertainties at global and regional scales. Differences in <span class="inline-formula">CH<sub>4</sub></span> isotopic source signatures <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> can help to constrain different source contributions (e.g., fossil, waste, agriculture). The Upper Silesian Coal Basin (USCB) represents one of the largest European <span class="inline-formula">CH<sub>4</sub></span> emission regions, with more than 500 <span class="inline-formula">Gg CH<sub>4</sub> yr<sup>−1</sup></span> released from more than 50 coal mine ventilation shafts, landfills, and wastewater treatment plants. During the CoMet (Carbon Dioxide and Methane Mission) campaign in June 2018 methane observations were conducted from a variety of platforms including aircraft and cars to quantify these emissions. Besides the continuous sampling of atmospheric methane concentration, numerous air samples were taken from inside and around the ventilation shafts (1–2 km distance) and aboard the <i>High Altitude and Long Range Research Aircraft</i> (<i>HALO</i>) and DLR Cessna Caravan aircraft, and they were analyzed in the laboratory for the isotopic composition of <span class="inline-formula">CH<sub>4</sub></span>.</p> <p>The airborne samples downwind of the USCB contained methane from the entire region and thus enabled determining the mean signature of the USCB accurately. This mean isotopic signature of methane emissions was <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M9" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">50.9</mn><mo>±</mo><mn mathvariant="normal">0.7</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="58pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="a27e853300f83c7b4b62be35f9825060"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00001.svg" width="58pt" height="10pt" src="acp-23-15749-2023-ie00001.png"/></svg:svg></span></span> ‰ for <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M11" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">226</mn><mo>±</mo><mn mathvariant="normal">9</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="46pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="4896105601a81a208b2037917e9548d2"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00002.svg" width="46pt" height="10pt" src="acp-23-15749-2023-ie00002.png"/></svg:svg></span></span> ‰ for <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>. This is in the range of previous USCB studies based on samples taken within the mines for <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> but more depleted in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> than reported before. Signatures of methane enhancements sampled upwind of the mines and in the free troposphere clearly showed the influence of biogenic sources. We determined the source signatures of individual coal mine ventilation shafts using ground-based samples. These signatures displayed a considerable range between different mines and also varied for individual shafts from day to day. Different layers of the USCB coal contain thermogenic methane, isotopically similar to natural gas, and methane formed through biogenic carbonate reduction. The signatures vary depending on what layer of coal is mined at the time of sampling. Mean shaft signatures range from <span class="inline-formula">−</span>60 ‰ to <span class="inline-formula">−</span>42 ‰ for <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and from <span class="inline-formula">−</span>200 ‰ to <span class="inline-formula">−</span>160 ‰ for <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>. A gradient in the signatures of subregions of the USCB is reflected both in the aircraft data and in the ground samples, with emissions from the southwest being most depleted in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> and emissions from the south being most depleted in <span class="inline-formula"><i>δ</i><sup>13</sup>C</span>, which is probably associated with the structural<span id="page15750"/> and lithostratigraphic history of the USCB and generation and migration processes of methane in the coal. The average signature of <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M23" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">49.8</mn><mo>±</mo><mn mathvariant="normal">5.7</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="58pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="c758e6ea1b22e7cd63c215ef195ab0da"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00003.svg" width="58pt" height="10pt" src="acp-23-15749-2023-ie00003.png"/></svg:svg></span></span> ‰ in <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> and <span class="inline-formula"><math xmlns="http://www.w3.org/1998/Math/MathML" id="M25" display="inline" overflow="scroll" dspmath="mathml"><mrow><mo>-</mo><mn mathvariant="normal">184</mn><mo>±</mo><mn mathvariant="normal">32</mn></mrow></math><span><svg:svg xmlns:svg="http://www.w3.org/2000/svg" width="52pt" height="10pt" class="svg-formula" dspmath="mathimg" md5hash="3b4d5869550ea9083ee077728cf29fbd"><svg:image xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="acp-23-15749-2023-ie00004.svg" width="52pt" height="10pt" src="acp-23-15749-2023-ie00004.png"/></svg:svg></span></span> ‰ in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> from the ventilation shafts clearly differs from the USCB regional signature in <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>. This makes a source attribution using <span class="inline-formula"><i>δ</i><sup>2</sup>H</span> signatures possible, which would not be possible with only the <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> isotopic signatures. We assume that the USCB plume mainly contains fossil coal mine methane and biogenic methane from waste treatment, because the USCB is a highly industrialized region with few other possible methane sources. Assuming a biogenic methane signature between and <span class="inline-formula">−</span>320 ‰ and <span class="inline-formula">−</span>280 ‰ for <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>, the biogenic methane emissions from the USCB account for 15 %–50 % of total emissions. The uncertainty range shows the need of comprehensive and extensive sampling from all possible source sectors for source apportionment. The share of anthropogenic–biogenic emissions of 0.4 %–14 % from this densely populated industrial region is underestimated in commonly used emission inventories. Generally, this study demonstrates the importance of <span class="inline-formula"><i>δ</i><sup>2</sup>H</span>-<span class="inline-formula">CH<sub>4</sub></span> observations for methane source apportionment in regions with a mix of thermogenic and biogenic sources and, especially in our case, where the <span class="inline-formula"><i>δ</i><sup>13</sup>C</span> signature of the coal mine gas has a large variability.</p>https://acp.copernicus.org/articles/23/15749/2023/acp-23-15749-2023.pdf |
| spellingShingle | A. Fiehn M. Eckl J. Kostinek M. Gałkowski M. Gałkowski C. Gerbig M. Rothe T. Röckmann M. Menoud M. Menoud H. Maazallahi M. Schmidt P. Korbeń J. Neçki M. Stanisavljević M. Stanisavljević J. Swolkień A. Fix A. Roiger Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures Atmospheric Chemistry and Physics |
| title | Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures |
| title_full | Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures |
| title_fullStr | Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures |
| title_full_unstemmed | Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures |
| title_short | Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures |
| title_sort | source apportionment of methane emissions from the upper silesian coal basin using isotopic signatures |
| url | https://acp.copernicus.org/articles/23/15749/2023/acp-23-15749-2023.pdf |
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