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  • 11
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 23, No. 4 ( 2023-02-27), p. 2699-2728
    Kurzfassung: Abstract. Power plants and large industrial facilities contribute more than half of global anthropogenic CO2 emissions. Quantifying the emissions of these point sources is therefore one of the main goals of the planned constellation of anthropogenic CO2 monitoring satellites (CO2M) of the European Copernicus program. Atmospheric transport models may be used to study the capabilities of such satellites through observing system simulation experiments and to quantify emissions in an inverse modeling framework. How realistically the CO2 plumes of power plants can be simulated and how strongly the results may depend on model type and resolution, however, is not well known due to a lack of observations available for benchmarking. Here, we use the unique data set of aircraft in situ and remote sensing observations collected during the CoMet (Carbon Dioxide and Methane Mission) measurement campaign downwind of the coal-fired power plants at Bełchatów in Poland and Jänschwalde in Germany in 2018 to evaluate the simulations of six different atmospheric transport models. The models include three large-eddy simulation (LES) models, two mesoscale numerical weather prediction (NWP) models extended for atmospheric tracer transport, and one Lagrangian particle dispersion model (LPDM) and cover a wide range of model resolutions from 200 m to 2 km horizontal grid spacing. At the time of the aircraft measurements between late morning and early afternoon, the simulated plumes were slightly (at Jänschwalde) to highly (at Bełchatów) turbulent, consistent with the observations, and extended over the whole depth of the atmospheric boundary layer (ABL; up to 1800 m a.s.l. (above sea level) in the case of Bełchatów). The stochastic nature of turbulent plumes puts fundamental limitations on a point-by-point comparison between simulations and observations. Therefore, the evaluation focused on statistical properties such as plume amplitude and width as a function of distance from the source. LES and NWP models showed similar performance and sometimes remarkable agreement with the observations when operated at a comparable resolution. The Lagrangian model, which was the only model driven by winds observed from the aircraft, quite accurately captured the location of the plumes but generally underestimated their width. A resolution of 1 km or better appears to be necessary to realistically capture turbulent plume structures. At a coarser resolution, the plumes disperse too quickly, especially in the near-field range (0–8 km from the source), and turbulent structures are increasingly smoothed out. Total vertical columns are easier to simulate accurately than the vertical distribution of CO2, since the latter is critically affected by profiles of vertical stability, especially near the top of the ABL. Cross-sectional flux and integrated mass enhancement methods applied to synthetic CO2M data generated from the model simulations with a random noise of 0.5–1.0 ppm (parts per million) suggest that emissions from a power plant like Bełchatów can be estimated with an accuracy of about 20 % from single overpasses. Estimates of the effective wind speed are a critical input for these methods. Wind speeds in the middle of the ABL appear to be a good approximation for plumes in a well-mixed ABL, as encountered during CoMet.
    Materialart: Online-Ressource
    ISSN: 1680-7324
    Sprache: Englisch
    Verlag: Copernicus GmbH
    Publikationsdatum: 2023
    ZDB Id: 2092549-9
    ZDB Id: 2069847-1
    Standort Signatur Einschränkungen Verfügbarkeit
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  • 12
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 23 ( 2021-12-01), p. 17345-17371
    Kurzfassung: Abstract. Methane (CH4) is the second most important anthropogenic greenhouse gas, whose atmospheric concentration is modulated by human-induced activities, and it has a larger global warming potential than carbon dioxide (CO2). Because of its short atmospheric lifetime relative to that of CO2, the reduction of the atmospheric abundance of CH4 is an attractive target for short-term climate mitigation strategies. However, reducing the atmospheric CH4 concentration requires a reduction of its emissions and, therefore, knowledge of its sources. For this reason, the CO2 and Methane (CoMet) campaign in May and June 2018 assessed emissions of one of the largest CH4 emission hot spots in Europe, the Upper Silesian Coal Basin (USCB) in southern Poland, using top-down approaches and inventory data. In this study, we will focus on CH4 column anomalies retrieved from spectral radiance observations, which were acquired by the 1D nadir-looking passive remote sensing Methane Airborne MAPper (MAMAP) instrument, using the weighting-function-modified differential optical absorption spectroscopy (WFM-DOAS) method. The column anomalies, combined with wind lidar measurements, are inverted to cross-sectional fluxes using a mass balance approach. With the help of these fluxes, reported emissions of small clusters of coal mine ventilation shafts are then assessed. The MAMAP CH4 column observations enable an accurate assignment of observed fluxes to small clusters of ventilation shafts. CH4 fluxes are estimated for four clusters with a total of 23 ventilation shafts, which are responsible for about 40 % of the total CH4 mining emissions in the target area. The observations were made during several overflights on different days. The final average CH4 fluxes for the single clusters (or sub-clusters) range from about 1 to 9 t CH4 h−1 at the time of the campaign. The fluxes observed at one cluster during different overflights vary by as much as 50 % of the average value. Associated errors (1σ) are usually between 15 % and 59 % of the average flux, depending mainly on the prevailing wind conditions, the number of flight tracks, and the magnitude of the flux itself. Comparison to known hourly emissions, where available, shows good agreement within the uncertainties. If only emissions reported annually are available for comparison with the observations, caution is advised due to possible fluctuations in emissions during a year or even within hours. To measure emissions even more precisely and to break them down further for allocation to individual shafts in a complex source region such as the USCB, imaging remote sensing instruments are recommended.
    Materialart: Online-Ressource
    ISSN: 1680-7324
    Sprache: Englisch
    Verlag: Copernicus GmbH
    Publikationsdatum: 2021
    ZDB Id: 2092549-9
    ZDB Id: 2069847-1
    Standort Signatur Einschränkungen Verfügbarkeit
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  • 13
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 21 ( 2020-11-03), p. 12675-12695
    Kurzfassung: Abstract. A severe reduction of greenhouse gas emissions is necessary to reach the objectives of the Paris Agreement. The implementation and continuous evaluation of mitigation measures requires regular independent information on emissions of the two main anthropogenic greenhouse gases, carbon dioxide (CO2) and methane (CH4). Our aim is to employ an observation-based method to determine regional-scale greenhouse gas emission estimates with high accuracy. We use aircraft- and ground-based in situ observations of CH4, CO2, carbon monoxide (CO), and wind speed from two research flights over the Upper Silesian Coal Basin (USCB), Poland, in summer 2018. The flights were performed as a part of the Carbon Dioxide and Methane (CoMet) mission above this European CH4 emission hot-spot region. A kriging algorithm interpolates the observed concentrations between the downwind transects of the trace gas plume, and then the mass flux through this plane is calculated. Finally, statistic and systematic uncertainties are calculated from measurement uncertainties and through several sensitivity tests, respectively. For the two selected flights, the in-situ-derived annual CH4 emission estimates are 13.8±4.3 and 15.1±4.0 kg s−1, which are well within the range of emission inventories. The regional emission estimates of CO2, which were determined to be 1.21±0.75 and 1.12±0.38 t s−1, are in the lower range of emission inventories. CO mass balance emissions of 10.1±3.6 and 10.7±4.4 kg s−1 for the USCB are slightly higher than the emission inventory values. The CH4 emission estimate has a relative error of 26 %–31 %, the CO2 estimate of 37 %–62 %, and the CO estimate of 36 %–41 %. These errors mainly result from the uncertainty of atmospheric background mole fractions and the changing planetary boundary layer height during the morning flight. In the case of CO2, biospheric fluxes also add to the uncertainty and hamper the assessment of emission inventories. These emission estimates characterize the USCB and help to verify emission inventories and develop climate mitigation strategies.
    Materialart: Online-Ressource
    ISSN: 1680-7324
    Sprache: Englisch
    Verlag: Copernicus GmbH
    Publikationsdatum: 2020
    ZDB Id: 2092549-9
    ZDB Id: 2069847-1
    Standort Signatur Einschränkungen Verfügbarkeit
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  • 14
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 7 ( 2022-04-04), p. 4303-4322
    Kurzfassung: Abstract. The oil and gas (O&G) sector is a significant source of methane (CH4) emissions. Quantifying these emissions remains challenging, with many studies highlighting discrepancies between measurements and inventory-based estimates. In this study, we present CH4 emission fluxes from 21 offshore O&G facilities collected in 10 O&G fields over two regions of the Norwegian continental shelf in 2019. Emissions of CH4 derived from measurements during 13 aircraft surveys were found to range from 2.6 to 1200 t yr−1 (with a mean of 211 t yr−1 across all 21 facilities). Comparing this with aggregated operator-reported facility emissions for 2019, we found excellent agreement (within 1σ uncertainty), with mean aircraft-measured fluxes only 16 % lower than those reported by operators. We also compared aircraft-derived fluxes with facility fluxes extracted from a global gridded fossil fuel CH4 emission inventory compiled for 2016. We found that the measured emissions were 42 % larger than the inventory for the area covered by this study, for the 21 facilities surveyed (in aggregate). We interpret this large discrepancy not to reflect a systematic error in the operator-reported emissions, which agree with measurements, but rather the representativity of the global inventory due to the methodology used to construct it and the fact that the inventory was compiled for 2016 (and thus not representative of emissions in 2019). This highlights the need for timely and up-to-date inventories for use in research and policy. The variable nature of CH4 emissions from individual facilities requires knowledge of facility operational status during measurements for data to be useful in prioritising targeted emission mitigation solutions. Future surveys of individual facilities would benefit from knowledge of facility operational status over time. Field-specific aggregated emissions (and uncertainty statistics), as presented here for the Norwegian Sea, can be meaningfully estimated from intensive aircraft surveys. However, field-specific estimates cannot be reliably extrapolated to other production fields without their own tailored surveys, which would need to capture a range of facility designs, oil and gas production volumes, and facility ages. For year-on-year comparison to annually updated inventories and regulatory emission reporting, analogous annual surveys would be needed for meaningful top-down validation. In summary, this study demonstrates the importance and accuracy of detailed, facility-level emission accounting and reporting by operators and the use of airborne measurement approaches to validate bottom-up accounting.
    Materialart: Online-Ressource
    ISSN: 1680-7324
    Sprache: Englisch
    Verlag: Copernicus GmbH
    Publikationsdatum: 2022
    ZDB Id: 2092549-9
    ZDB Id: 2069847-1
    Standort Signatur Einschränkungen Verfügbarkeit
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  • 15
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 17, No. 11 ( 2017-06-08), p. 6723-6741
    Kurzfassung: Abstract. Halogenated very short-lived substances (VSLSs) are naturally produced in the ocean and emitted to the atmosphere. When transported to the stratosphere, these compounds can have a significant influence on the ozone layer and climate. During a research cruise on RV Sonne in the subtropical and tropical west Indian Ocean in July and August 2014, we measured the VSLSs, methyl iodide (CH3I) and for the first time bromoform (CHBr3) and dibromomethane (CH2Br2), in surface seawater and the marine atmosphere to derive their emission strengths. Using the Lagrangian particle dispersion model FLEXPART with ERA-Interim meteorological fields, we calculated the direct contribution of observed VSLS emissions to the stratospheric halogen burden during the Asian summer monsoon. Furthermore, we compare the in situ calculations with the interannual variability of transport from a larger area of the west Indian Ocean surface to the stratosphere for July 2000–2015. We found that the west Indian Ocean is a strong source for CHBr3 (910 pmol m−2 h−1), very strong source for CH2Br2 (930 pmol m−2 h−1), and an average source for CH3I (460 pmol m−2 h−1). The atmospheric transport from the tropical west Indian Ocean surface to the stratosphere experiences two main pathways. On very short timescales, especially relevant for the shortest-lived compound CH3I (3.5 days lifetime), convection above the Indian Ocean lifts oceanic air masses and VSLSs towards the tropopause. On a longer timescale, the Asian summer monsoon circulation transports oceanic VSLSs towards India and the Bay of Bengal, where they are lifted with the monsoon convection and reach stratospheric levels in the southeastern part of the Asian monsoon anticyclone. This transport pathway is more important for the longer-lived brominated compounds (17 and 150 days lifetime for CHBr3 and CH2Br2). The entrainment of CHBr3 and CH3I from the west Indian Ocean to the stratosphere during the Asian summer monsoon is lower than from previous cruises in the tropical west Pacific Ocean during boreal autumn and early winter but higher than from the tropical Atlantic during boreal summer. In contrast, the projected CH2Br2 entrainment was very high because of the high emissions during the west Indian Ocean cruise. The 16-year July time series shows highest interannual variability for the shortest-lived CH3I and lowest for the longest-lived CH2Br2. During this time period, a small increase in VSLS entrainment from the west Indian Ocean through the Asian monsoon to the stratosphere is found. Overall, this study confirms that the subtropical and tropical west Indian Ocean is an important source region of halogenated VSLSs, especially CH2Br2, to the troposphere and stratosphere during the Asian summer monsoon.
    Materialart: Online-Ressource
    ISSN: 1680-7324
    Sprache: Englisch
    Verlag: Copernicus GmbH
    Publikationsdatum: 2017
    ZDB Id: 2092549-9
    ZDB Id: 2069847-1
    Standort Signatur Einschränkungen Verfügbarkeit
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