Atmospheric methane (CH4) concentrations have more than doubled since the beginning of the industrial age, making CH4 the second most important anthropogenic greenhouse gas after carbon dioxide ...(CO2). The oil and gas sector represents one of the major anthropogenic CH4 emitters as it is estimated to account for 22 % of global anthropogenic CH4 emissions. An airborne field campaign was conducted in April–May 2019 to study CH4 emissions from offshore gas facilities in the southern North Sea with the aim of deriving emission estimates using a top-down (measurement-led) approach. We present CH4 fluxes for six UK and five Dutch offshore platforms or platform complexes using the well-established mass balance flux method. We identify specific gas production emissions and emission processes (venting and fugitive or flaring and combustion) using observations of co-emitted ethane (C2H6) and CO2. We compare our top-down estimated fluxes with a ship-based top-down study in the Dutch sector and with bottom-up estimates from a globally gridded annual inventory, UK national annual point-source inventories, and operator-based reporting for individual Dutch facilities. In this study, we find that all the inventories, except for the operator-based facility-level reporting, underestimate measured emissions, with the largest discrepancy observed with the globally gridded inventory. Individual facility reporting, as available for Dutch sites for the specific survey date, shows better agreement with our measurement-based estimates. For all the sampled Dutch installations together, we find that our estimated flux of (122.9 ± 36.8) kg h−1 deviates by a factor of 0.64 (0.33–12) from reported values (192.8 kg h−1). Comparisons with aircraft observations in two other offshore regions (the Norwegian Sea and the Gulf of Mexico) show that measured, absolute facility-level emission rates agree with the general distribution found in other offshore basins despite different production types (oil, gas) and gas production rates, which vary by 2 orders of magnitude. Therefore, mitigation is warranted equally across geographies.
During the ACCESS airborne campaign in July 2012, extensive boreal forest fires resulted in significant aerosol transport to the Arctic. A 10-day episode combining intense biomass burning over ...Siberia and low-pressure systems over the Arctic Ocean resulted in efficient transport of plumes containing black carbon (BC) towards the Arctic, mostly in the upper troposphere (6–8 km). A combination of in situ observations (DLR Falcon aircraft), satellite analysis and WRF-Chem simulations is used to understand the vertical and horizontal transport mechanisms of BC with a focus on the role of wet removal. Between the northwestern Norwegian coast and the Svalbard archipelago, the Falcon aircraft sampled plumes with enhanced CO concentrations up to 200 ppbv and BC mixing ratios up to 25 ng kg−1. During transport to the Arctic region, a large fraction of BC particles are scavenged by two wet deposition processes, namely wet removal by large-scale precipitation and removal in wet convective updrafts, with both processes contributing almost equally to the total accumulated deposition of BC. Our results underline that applying a finer horizontal resolution (40 instead of 100 km) improves the model performance, as it significantly reduces the overestimation of BC levels observed at a coarser resolution in the mid-troposphere. According to the simulations at 40 km, the transport efficiency of BC (TEBC) in biomass burning plumes was larger (60 %), because it was impacted by small accumulated precipitation along trajectory (1 mm). In contrast TEBC was small (< 30 %) and accumulated precipitation amounts were larger (5–10 mm) in plumes influenced by urban anthropogenic sources and flaring activities in northern Russia, resulting in transport to lower altitudes. TEBC due to large-scale precipitation is responsible for a sharp meridional gradient in the distribution of BC concentrations. Wet removal in cumulus clouds is the cause of modeled vertical gradient of TEBC, especially in the mid-latitudes, reflecting the distribution of convective precipitation, but is dominated in the Arctic region by the large-scale wet removal associated with the formation of stratocumulus clouds in the planetary boundary layer (PBL) that produce frequent drizzle.
Methane (CH4) emissions from coal production amount to roughly one-third of European anthropogenic CH4 emissions in the atmosphere. Poland is the largest hard coal producer in the European Union with ...the Polish side of the Upper Silesian Coal Basin (USCB) as the main part of it. Emission estimates for CH4 from the USCB for individual coal mine ventilation shafts range between 0.03 and 20 kt a−1, amounting to a basin total of roughly 440 kt a−1 according to the European Pollutant Release and Transfer Register (E-PRTR, http://prtr.ec.europa.eu/, 2014). We mounted a ground-based, portable, sun-viewing FTS (Fourier transform spectrometer) on a truck for sampling coal mine ventilation plumes by driving cross-sectional stop-and-go patterns at 1 to 3 km from the exhaust shafts. Several of these transects allowed for estimation of CH4 emissions based on the observed enhancements of the column-averaged dry-air mole fractions of methane (XCH4) using a mass balance approach. Our resulting emission estimates range from 6±1 kt a−1 for a single shaft up to 109±33 kt a−1 for a subregion of the USCB, which is in broad agreement with the E-PRTR reports. Three wind lidars were deployed in the larger USCB region providing ancillary information about spatial and temporal variability of wind and turbulence in the atmospheric boundary layer. Sensitivity studies show that, despite drawing from the three wind lidars, the uncertainty of the local wind dominates the uncertainty of the emission estimates, by far exceeding errors related to the XCH4 measurements themselves. Wind-related relative errors on the emission estimates typically amount to 20 %.
The UNFCCC (United Nations Framework Convention on Climate Change) requires the nations of the world to report their carbon dioxide (CO2) emissions. The independent verification of these reported ...emissions is a cornerstone for advancing towards the emission accounting and reduction measures agreed upon in the Paris Agreement. In this paper, we present the concept and first performance assessment of a compact spaceborne imaging spectrometer with a spatial resolution of 50×50 m2 that could contribute to the “monitoring, verification and reporting” (MVR) of CO2 emissions worldwide. CO2 emissions from medium-sized power plants (1–10 MtCO2yr-1), currently not targeted by other spaceborne missions, represent a significant part of the global CO2 emission budget. In this paper we show that the proposed instrument concept is able to resolve emission plumes from such localized sources as a first step towards corresponding CO2 flux estimates.Through radiative transfer simulations, including a realistic instrument noise model and a global trial ensemble covering various geophysical scenarios, it is shown that an instrument noise error of 1.1 ppm (1σ) can be achieved for the retrieval of the column-averaged dry-air mole fraction of CO2 (XCO2). Despite a limited amount of information from a single spectral window and a relatively coarse spectral resolution, scattering by atmospheric aerosol and cirrus can be partly accounted for in the XCO2 retrieval, with deviations of at most 4.0 ppm from the true abundance for two-thirds of the scenes in the global trial ensemble.We further simulate the ability of the proposed instrument concept to observe CO2 plumes from single power plants in an urban area using high-resolution CO2 emission and surface albedo data for the city of Indianapolis. Given the preliminary instrument design and the corresponding instrument noise error, emission plumes from point sources with an emission rate down to the order of 0.3 MtCO2yr-1 can be resolved, i.e., well below the target source strength of 1 MtCO2yr-1. This leaves a significant margin for additional error sources, like scattering particles and complex meteorology, and shows the potential for subsequent CO2 flux estimates with the proposed instrument concept.
ARCTIC AIR POLLUTION Law, Katharine S.; Stohl, Andreas; Quinn, Patricia K. ...
Bulletin of the American Meteorological Society,
12/2014, Letnik:
95, Številka:
12
Journal Article
Recenzirano
Odprti dostop
Given the rapid nature of climate change occurring in the Arctic and the difficulty climate models have in quantitatively reproducing observed changes such as sea ice loss, it is important to improve ...understanding of the processes leading to climate change in this region, including the role of short-lived climate pollutants such as aerosols and ozone. It has long been known that pollution produced from emissions at midlatitudes can be transported to the Arctic, resulting in a winter/spring aerosol maximum known as Arctic haze. However, many uncertainties remain about the composition and origin of Arctic pollution throughout the troposphere; for example, many climate–chemistry models fail to reproduce the strong seasonality of aerosol abundance observed at Arctic surface sites, the origin and deposition mechanisms of black carbon (soot) particles that darken the snow and ice surface in the Arctic is poorly understood, and chemical processes controlling the abundance of tropospheric ozone are not well quantified. The International Polar Year (IPY) Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, Climate, Chemistry, Aerosols and Transport (POLARCAT) core project had the goal to improve understanding about the origins of pollutants transported to the Arctic; to detail the chemical composition, optical properties, and climate forcing potential of Arctic aerosols; to evaluate the processes governing tropospheric ozone; and to quantify the role of boreal forest fires. This article provides a review of the many results now available based on analysis of data collected during the POLARCAT aircraft-, ship-, and ground-based field campaigns in spring and summer 2008. Major findings are highlighted and areas requiring further investigation are discussed.
Celotno besedilo
Dostopno za:
BFBNIB, DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
Tunable laser direct absorption spectroscopy is a widely used technique for the in situ sensing of atmospheric composition. Aircraft deployment poses a challenging operating environment for ...instruments measuring climatologically relevant gases in the Earth's atmosphere. Here, we demonstrate the successful adaption of a commercially available continuous wave quantum cascade laser (QCL) and interband cascade laser (ICL) based spectrometer for airborne in situ trace gas measurements with a local to regional focus. The instrument measures methane, ethane, carbon dioxide, carbon monoxide, nitrous oxide and water vapor simultaneously, with high 1 s–1σ precision (740 ppt, 205 ppt, 460 ppb, 2.2 ppb, 137 ppt and 16 ppm, respectively) and high frequency (2 Hz). We estimate a total 1 s–1σ uncertainty of 1.85 ppb, 1.6 ppb, 1.0 ppm, 7.0 ppb and 0.8 ppb in CH4, C2H6, CO2, CO and N2O, respectively. The instrument enables simultaneous and continuous observations for all targeted species. Frequent calibration allows for a measurement duty cycle≥90 %. Custom retrieval software has been implemented and instrument performance is reported for a first field deployment during NASA's Atmospheric Carbon and Transport – America (ACT-America) campaign in fall 2017 over the eastern and central USA. This includes an inter-instrumental comparison with a calibrated cavity ring-down greenhouse gas analyzer (operated by NASA Langley Research Center, Hampton, USA) and periodic flask samples analyzed at the National Oceanic and Atmospheric Administration (NOAA). We demonstrate good agreement of the QCL- and ICL-based instrument to these concurrent observations within the combined measurement uncertainty after correcting for a constant bias. We find that precise knowledge of theδ13C of the working standards and the sampled air is needed to enhance CO2 compatibility when operating on the 2227.604 cm-1 13C16O2 absorption line.
Methane is the second most important greenhouse gas in terms of anthropogenic radiative forcing. Since pre-industrial times, the globally averaged dry mole fraction of methane in the atmosphere has ...increased considerably. Emissions from coal mining are one of the primary anthropogenic methane sources. However, our knowledge about different sources and sinks of methane is still subject to great uncertainties. Comprehensive measurement campaigns and reliable chemistry–climate models, are required to fully understand the global methane budget and to further develop future climate mitigation strategies. The CoMet 1.0 campaign (May to June 2018) combined airborne in situ, as well as passive and active remote sensing measurements to quantify the emissions from coal mining in the Upper Silesian Coal Basin (USCB, Poland). Roughly 502 kt of methane is emitted from the ventilation shafts per year. In order to help with the flight planning during the campaigns, we performed 6 d forecasts using the online coupled, three-time nested global and regional chemistry–climate model MECO(n). We applied three-nested COSMO/MESSy instances going down to a spatial resolution of 2.8 km over the USCB. The nested global–regional model system allows for the separation of local emission contributions from fluctuations in the background methane. Here, we introduce the forecast set-up and assess the impact of the model's spatial resolution on the simulation of methane plumes from the ventilation shafts. Uncertainties in simulated methane mixing ratios are estimated by comparing different airborne measurements to the simulations. Results show that MECO(3) is able to simulate the observed methane plumes and the large-scale patterns (including vertically integrated values) reasonably well. Furthermore, we obtain reasonable forecast results up to forecast day four.
In the last decade, much work has been done to better understand methane (CH4) emissions from the oil and gas (O&G) industry in the United States. Ethane (C2H6), a gas that is co‐emitted with ...thermogenic sources of CH4, is emitted in the US predominantly by the O&G sector. In this study, we perform an inverse analysis on 200 h of atmospheric boundary layer C2H6 measurements to estimate C2H6 emissions from the US O&G sector. Measurements were collected from 2017 to 2019 as part of the Atmospheric Carbon and Transport (ACT) America aircraft campaign and encompass much of the central and eastern United States. We find that for the fall, winter, and spring campaigns, C2H6 data consistently exceeds values that would be expected based on EPA O&G leak rate estimates by more than 50%. C2H6 observations from the summer 2019 data set show significantly lower C2H6 enhancements in the southcentral region that cannot be reconciled with data from the other three seasons, either due to complex meteorological conditions or a temporal shift in the emissions. Combining the fall, winter, and spring C2H6 posterior emissions estimate to an inventory of O&G CH4 emissions, we estimate that O&G CH4 emissions are larger than EPA inventory values by 48%–76%. Uncertainties in the gas composition data limit the accuracy of using C2H6 as a proxy for O&G CH4 emissions. These limits could be resolved retroactively by increasing the availability of industry‐collected gas composition data.
Plain Language SummaryMethane is a potent greenhouse gas responsible for a quarter of the warming the climate has experienced thus far. The oil and gas (O&G) sector is a significant source of methane through leaks in its infrastructure. Recent studies of individual basins have found emissions from O&G in the US to be greater than inventory estimates, but difficulties arise with source attribution in broader scale studies due to the numerous potential sources of methane. This study quantifies methane emissions from O&G by looking at atmospheric ethane, a gas whose emissions originate mostly from O&G in the US. Hundreds of hours of boundary layer ethane observations were collected via aircraft over the course of four seasons between 2017 and 2019. These observations are compared with model‐projected ethane values based on our current knowledge of ethane emissions, and those emissions are adjusted to best match the observed data. We find ethane emissions are grossly underestimated in the US. Because ethane is co‐emitted with O&G methane sources, this underestimation of ethane reflects similar underestimations in O&G methane emissions. We conclude that US inventories are underestimating methane emissions from O&G by 48%–76%.
Key PointsThis study uses ethane observations to quantify both ethane and methane emissions from the United States oil and gas (O&G) sectorEthane emissions in the southcentral and eastern United States are larger than the NEI 2017 inventory by more than a factor of 2Ethane results indicate that the US EPA methane inventory is underestimating leak rates from the O&G sector
Verifying anthropogenic carbon dioxide (CO2) emissions globally is essential to inform about the progress of institutional efforts to mitigate anthropogenic climate forcing. To monitor localized ...emission sources, spectroscopic satellite sensors have been proposed that operate on the CO2 absorption bands in the shortwave-infrared (SWIR) spectral range with ground resolution as fine as a few tens of meters to about a hundred meters. When designing such sensors, fine ground resolution requires a trade-off towards coarse spectral resolution in order to achieve sufficient noise performance. Since fine ground resolution also implies limited ground coverage, such sensors are envisioned to fly in fleets of satellites, requiring low-cost and simple design, e.g., by restricting the spectrometer to a single spectral band.Here, we use measurements of the Greenhouse Gases Observing Satellite (GOSAT) to evaluate the spectral resolution and spectral band selection of a prospective satellite sensor with fine ground resolution. To this end, we degrade GOSAT SWIR spectra of the CO2 bands at 1.6 (SWIR-1) and 2.0 µm (SWIR-2) to coarse spectral resolution, without a further addition of noise, and we evaluate single-band retrievals of the column-averaged dry-air mole fractions of CO2 (XCO2) by comparison to ground truth provided by the Total Carbon Column Observing Network (TCCON) and by comparison to global “native” GOSAT retrievals with native spectral resolution and spectral band selection. Coarsening spectral resolution from GOSAT's native resolving power of >20000 to the range of 700 to a few thousand makes the scatter of differences between the SWIR-1 and SWIR-2 retrievals and TCCON increase moderately. For resolving powers of 1200 (SWIR-1) and 1600 (SWIR-2), the scatter increases from 2.4 (native) to 3.0 ppm for SWIR-1 and 3.3 ppm for SWIR-2. Coarser spectral resolution yields only marginally worse performance than the native GOSAT configuration in terms of station-to-station variability and geophysical parameter correlations for the GOSAT–TCCON differences. Comparing the SWIR-1 and SWIR-2 configurations to native GOSAT retrievals on the global scale, however, reveals that the coarse-resolution SWIR-1 and SWIR-2 configurations suffer from some spurious correlations with geophysical parameters that characterize the light-scattering properties of the scene such as particle amount, size, height and surface albedo. Overall, the SWIR-1 and SWIR-2 configurations with resolving powers of 1200 and 1600 show promising performance for future sensor design in terms of random error sources while residual errors induced by light scattering along the light path need to be investigated further. Due to the stronger CO2 absorption bands in SWIR-2 than in SWIR-1, the former has the advantage that measurement noise propagates less into the retrieved XCO2 and that some retrieval information on particle scattering properties is accessible.
Column-averaged dry-air mole fractions of carbon dioxide (XCO2) and methane (XCH4) measured by a solar viewing portable Fourier transform spectrometer (FTS, EM27/SUN) have been characterized and ...validated by comparison using in situ profile measurements made during the transfer flights of two aircraft campaigns: Korea-United States Air Quality Study (KORUS-AQ) and Effect of Megacities on the Transport and Transformation of Pollutants at Regional and Global Scales (EMeRGe). The aircraft flew over two Total Carbon Column Observing Network (TCCON) sites: Rikubetsu, Japan (43.46∘ N, 143.77∘ E), for the KORUS-AQ campaign and Burgos, Philippines (18.53∘ N, 120.65∘ E), for the EMeRGe campaign. The EM27/SUN was deployed at the corresponding TCCON sites during the overflights. The mole fraction profiles obtained by the aircraft over Rikubetsu differed between the ascending and the descending flights above approximately 8 km for both CO2 and CH4. Because the spatial pattern of tropopause heights based on potential vorticity values from the ERA5 reanalysis shows that the tropopause height over the Rikubetsu site was consistent with the descending profile, we used only the descending profile to compare with the EM27/SUN data. Both the XCO2 and XCH4 derived from the descending profiles over Burgos were lower than those from the ascending profiles. Output from the Weather Research and Forecasting Model indicates that higher CO2 for the ascending profile originated in central Luzon, an industrialized and densely populated region about 400 km south of the Burgos TCCON site. Air masses observed with the EM27/SUN overlap better with those from the descending aircraft profiles than those from the ascending aircraft profiles with respect to their properties such as origin and atmospheric residence times. Consequently, the descending aircraft profiles were used for the comparison with the EM27/SUN data. The EM27/SUN XCO2 and XCH4 data were derived by using the GGG2014 software without applying air-mass-independent correction factors (AICFs). The comparison of the EM27/SUN observations with the aircraft data revealed that, on average, the EM27/SUN XCO2 data were biased low by 1.22 % and the EM27/SUN XCH4 data were biased low by 1.71 %. The resulting AICFs of 0.9878 for XCO2 and 0.9829 for XCH4 were obtained for the EM27/SUN. Applying AICFs being utilized for the TCCON data (0.9898 forXCO2 and 0.9765 for XCH4) to the EM27/SUN data induces an underestimate for XCO2 and an overestimate for XCH4.
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