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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 13 ( 2021-07-14), p. 10527-10555
    Abstract: Abstract. In regions where there are multiple sources of methane (CH4) in close proximity, it can be difficult to apportion the CH4 measured in the atmosphere to the appropriate sources. In the Surat Basin, Queensland, Australia, coal seam gas (CSG) developments are surrounded by cattle feedlots, grazing cattle, piggeries, coal mines, urban centres and natural sources of CH4. The characterization of carbon (δ13C) and hydrogen (δD) stable isotopic composition of CH4 can help distinguish between specific emitters of CH4. However, in Australia there is a paucity of data on the various isotopic signatures of the different source types. This research examines whether dual isotopic signatures of CH4 can be used to distinguish between sources of CH4 in the Surat Basin. We also highlight the benefits of sampling at nighttime. During two campaigns in 2018 and 2019, a mobile CH4 monitoring system was used to detect CH4 plumes. Sixteen plumes immediately downwind from known CH4 sources (or individual facilities) were sampled and analysed for their CH4 mole fraction and δ13CCH4 and δDCH4 signatures. The isotopic signatures of the CH4 sources were determined using the Keeling plot method. These new source signatures were then compared to values documented in reports and peer-reviewed journal articles. In the Surat Basin, CSG sources have δ13CCH4 signatures between −55.6 ‰ and −50.9 ‰ and δDCH4 signatures between −207.1 ‰ and −193.8 ‰. Emissions from an open-cut coal mine have δ13CCH4 and δDCH4 signatures of -60.0±0.6 ‰ and -209.7±1.8 ‰ respectively. Emissions from two ground seeps (abandoned coal exploration wells) have δ13CCH4 signatures of -59.9±0.3 ‰ and -60.5±0.2 ‰ and δDCH4 signatures of -185.0±3.1 ‰ and -190.2±1.4 ‰. A river seep had a δ13CCH4 signature of -61.2±1.4 ‰ and a δDCH4 signature of -225.1±2.9 ‰. Three dominant agricultural sources were analysed. The δ13CCH4 and δDCH4 signatures of a cattle feedlot are -62.9±1.3 ‰ and -310.5±4.6 ‰ respectively, grazing (pasture) cattle have δ13CCH4 and δDCH4 signatures of -59.7±1.0 ‰ and -290.5±3.1 ‰ respectively, and a piggery sampled had δ13CCH4 and δDCH4 signatures of -47.6±0.2 ‰ and -300.1±2.6 ‰ respectively, which reflects emissions from animal waste. An export abattoir (meat works and processing) had δ13CCH4 and δDCH4 signatures of -44.5±0.2 ‰ and -314.6±1.8 ‰ respectively. A plume from a wastewater treatment plant had δ13CCH4 and δDCH4 signatures of -47.6±0.2 ‰ and -177.3±2.3 ‰ respectively. In the Surat Basin, source attribution is possible when both δ13CCH4 and δDCH4 are measured for the key categories of CSG, cattle, waste from feedlots and piggeries, and water treatment plants. Under most field situations using δ13CCH4 alone will not enable clear source attribution. It is common in the Surat Basin for CSG and feedlot facilities to be co-located. Measurement of both δ13CCH4 and δDCH4 will assist in source apportionment where the plumes from two such sources are mixed.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 2
    In: Elementa: Science of the Anthropocene, University of California Press, Vol. 10, No. 1 ( 2022-04-27)
    Abstract: Methane (CH4) emissions to the atmosphere from the oil and gas sector in Romania remain highly uncertain despite their relevance for the European Union’s goals to reduce greenhouse gas emissions. Measurements of CH4 isotopic composition can be used for source attribution, which is important in top-down studies of emissions from extended areas. We performed isotope measurements of CH4 in atmospheric air samples collected from an aircraft (24 locations) and ground vehicles (83 locations), around oil and gas production sites in Romania, with focus on the Romanian Plain. Ethane to methane ratios were derived at 412 locations of the same fossil fuel activity clusters. The resulting isotopic signals (δ13C and δ2H in CH4) covered a wide range of values, indicating mainly thermogenic gas sources (associated with oil production) in the Romanian Plain, mostly in Prahova county (δ13C from –67.8 ± 1.2 to –22.4 ± 0.04 ‰ Vienna Pee Dee Belmnite; δ2H from –255 ± 12 to –138 ± 11 ‰ Vienna Standard Mean Ocean Water) but also the presence of some natural gas reservoirs of microbial origin in Dolj, Ialomiţa, Prahova, and likely Teleorman counties. The classification based on ethane data was generally in agreement with the one based on CH4 isotopic composition and confirmed the interpretation of the gas origin. In several cases, CH4 enhancements sampled from the aircraft could directly be linked to the underlying production clusters using wind data. The combination of δ13C and δ2H signals in these samples confirms that the oil and gas production sector is the main source of CH4 emissions in the target areas. We found that average CH4 isotopic signatures in Romania are significantly lower than commonly used values for the global fossil fuel emissions. Our results emphasize the importance of regional variations in CH4 isotopes, with implications for global inversion modeling studies.
    Type of Medium: Online Resource
    ISSN: 2325-1026
    Language: English
    Publisher: University of California Press
    Publication Date: 2022
    detail.hit.zdb_id: 2745461-7
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 23 ( 2022-12-12), p. 15527-15558
    Abstract: Abstract. In-flight measurements of atmospheric methane (CH4(a)) and mass balance flux quantification studies can assist with verification and improvement in the UNFCCC National Inventory reported CH4 emissions. In the Surat Basin gas fields, Queensland, Australia, coal seam gas (CSG) production and cattle farming are two of the major sources of CH4 emissions into the atmosphere. Because of the rapid mixing of adjacent plumes within the convective boundary layer, spatially attributing CH4(a) mole fraction readings to one or more emission sources is difficult. The primary aims of this study were to use the CH4(a) isotopic composition (δ13CCH4(a)) of in-flight atmospheric air (IFAA) samples to assess where the bottom–up (BU) inventory developed specifically for the region was well characterised and to identify gaps in the BU inventory (missing sources or over- and underestimated source categories). Secondary aims were to investigate whether IFAA samples collected downwind of predominantly similar inventory sources were useable for characterising the isotopic signature of CH4 sources (δ13CCH4(s)) and to identify mitigation opportunities. IFAA samples were collected between 100–350 m above ground level (m a.g.l.) over a 2-week period in September 2018. For each IFAA sample the 2 h back-trajectory footprint area was determined using the NOAA HYSPLIT atmospheric trajectory modelling application. IFAA samples were gathered into sets, where the 2 h upwind BU inventory had 〉 50 % attributable to a single predominant CH4 source (CSG, grazing cattle, or cattle feedlots). Keeling models were globally fitted to these sets using multiple regression with shared parameters (background-air CH4(b) and δ13CCH4(b)). For IFAA samples collected from 250–350 m a.g.l. altitude, the best-fit δ13CCH4(s) signatures compare well with the ground observation: CSG δ13CCH4(s) of −55.4 ‰ (confidence interval (CI) 95 % ± 13.7 ‰) versus δ13CCH4(s) of −56.7 ‰ to −45.6 ‰; grazing cattle δ13CCH4(s) of −60.5 ‰ (CI 95 % ± 15.6 ‰) versus −61.7 ‰ to −57.5 ‰. For cattle feedlots, the derived δ13CCH4(s) (−69.6 ‰, CI 95 % ± 22.6 ‰), was isotopically lighter than the ground-based study (δ13CCH4(s) from −65.2 ‰ to −60.3 ‰) but within agreement given the large uncertainty for this source. For IFAA samples collected between 100–200 m a.g.l. the δ13CCH4(s) signature for the CSG set (−65.4 ‰, CI 95 % ± 13.3 ‰) was isotopically lighter than expected, suggesting a BU inventory knowledge gap or the need to extend the population statistics for CSG δ13CCH4(s) signatures. For the 100–200 m a.g.l. set collected over grazing cattle districts the δ13CCH4(s) signature (−53.8 ‰, CI 95 % ± 17.4 ‰) was heavier than expected from the BU inventory. An isotopically light set had a low δ13CCH4(s) signature of −80.2 ‰ (CI 95 % ± 4.7 ‰). A CH4 source with this low δ13CCH4(s) signature has not been incorporated into existing BU inventories for the region. Possible sources include termites and CSG brine ponds. If the excess emissions are from the brine ponds, they can potentially be mitigated. It is concluded that in-flight atmospheric δ13CCH4(a) measurements used in conjunction with endmember mixing modelling of CH4 sources are powerful tools for BU inventory verification.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 4
    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
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    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
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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