scholarly journals Estimating European volatile organic compound emissions using satellite observations of formaldehyde from the Ozone Monitoring Instrument

2010 ◽  
Vol 10 (8) ◽  
pp. 19697-19736 ◽  
Author(s):  
G. Curci ◽  
P. I. Palmer ◽  
T. P. Kurosu ◽  
K. Chance ◽  
G. Visconti

Abstract. Emission of non-methane Volatile Organic Compounds (VOCs) to the atmosphere stems from biogenic and human activities, and their estimation is difficult because of the many and not fully understood processes involved. In order to narrow down the uncertainty related to VOC emissions, which negatively reflects on our ability to simulate the atmospheric composition, we exploit satellite observations of formaldehyde (HCHO), an ubiquitous oxidation product of most VOCs, focusing on Europe. HCHO column observations from the Ozone Monitoring Instrument (OMI) reveal a marked seasonal cycle with a summer maximum and winter minimum. In summer, the oxidation of methane and other long-lived VOCs supply a slowly varying background HCHO column, while HCHO variability is dominated by most reactive VOC, primarily biogenic isoprene followed in importance by biogenic terpenes and anthropogenic VOCs. The chemistry-transport model CHIMERE qualitatively reproduces the temporal and spatial features of the observed HCHO column, but display regional biases which are attributed mainly to incorrect biogenic VOC emissions, calculated with the Model of Emissions of Gases and Aerosol from Nature (MEGAN) algorithm. These "bottom-up" or a-priori emissions are corrected through a Bayesian inversion of the OMI HCHO observations. Resulting "top-down" or a-posteriori isoprene emissions are lower than "bottom-up" by 40% over the Balkans and by 20% over Southern Germany, and higher by 20% over Iberian Peninsula, Greece and Italy. The inversion is shown to be robust against assumptions on the a-priori and the inversion parameters. We conclude that OMI satellite observations of HCHO can provide a quantitative "top-down" constraint on the European "bottom-up" VOC inventories.

2010 ◽  
Vol 10 (23) ◽  
pp. 11501-11517 ◽  
Author(s):  
G. Curci ◽  
P. I. Palmer ◽  
T. P. Kurosu ◽  
K. Chance ◽  
G. Visconti

Abstract. Emission of non-methane Volatile Organic Compounds (VOCs) to the atmosphere stems from biogenic and human activities, and their estimation is difficult because of the many and not fully understood processes involved. In order to narrow down the uncertainty related to VOC emissions, which negatively reflects on our ability to simulate the atmospheric composition, we exploit satellite observations of formaldehyde (HCHO), an ubiquitous oxidation product of most VOCs, focusing on Europe. HCHO column observations from the Ozone Monitoring Instrument (OMI) reveal a marked seasonal cycle with a summer maximum and winter minimum. In summer, the oxidation of methane and other long-lived VOCs supply a slowly varying background HCHO column, while HCHO variability is dominated by most reactive VOC, primarily biogenic isoprene followed in importance by biogenic terpenes and anthropogenic VOCs. The chemistry-transport model CHIMERE qualitatively reproduces the temporal and spatial features of the observed HCHO column, but display regional biases which are attributed mainly to incorrect biogenic VOC emissions, calculated with the Model of Emissions of Gases and Aerosol from Nature (MEGAN) algorithm. These "bottom-up" or a-priori emissions are corrected through a Bayesian inversion of the OMI HCHO observations. Resulting "top-down" or a-posteriori isoprene emissions are lower than "bottom-up" by 40% over the Balkans and by 20% over Southern Germany, and higher by 20% over Iberian Peninsula, Greece and Italy. We conclude that OMI satellite observations of HCHO can provide a quantitative "top-down" constraint on the European "bottom-up" VOC inventories.


2018 ◽  
Vol 18 (20) ◽  
pp. 15017-15046 ◽  
Author(s):  
Hansen Cao ◽  
Tzung-May Fu ◽  
Lin Zhang ◽  
Daven K. Henze ◽  
Christopher Chan Miller ◽  
...  

Abstract. We used the GEOS-Chem model and its adjoint to quantify Chinese non-methane volatile organic compound (NMVOC) emissions for the year 2007, using the tropospheric column concentrations of formaldehyde and glyoxal observed by the Global Ozone Monitoring Experiment 2A (GOME-2A) instrument and the Ozone Monitoring Instrument (OMI) as quantitative constraints. We conducted a series of inversion experiments using different combinations of satellite observations to explore their impacts on the top-down emission estimates. Our top-down estimates for Chinese annual total NMVOC emissions were 30.7 to 49.5 (average 41.9) Tg yr−1, including 16.4 to 23.6 (average 20.2) Tg yr−1 from anthropogenic sources, 12.2 to 22.8 (average 19.2) Tg yr−1 from biogenic sources, and 2.08 to 3.13 (average 2.48) Tg yr−1 from biomass burning. In comparison, the a priori estimate for Chinese annual total NMVOC emissions was 38.3 Tg yr−1, including 18.8 Tg yr−1 from anthropogenic sources, 17.3 Tg yr−1 from biogenic sources, and 2.27 Tg yr−1 from biomass burning. The simultaneous use of glyoxal and formaldehyde observations helped distinguish the NMVOC species from different sources and was essential in constraining anthropogenic emissions. Our four inversion experiments consistently showed that the Chinese anthropogenic emissions of NMVOC precursors of glyoxal were larger than the a priori estimates. Our top-down estimates for Chinese annual emission of anthropogenic aromatics (benzene, toluene, and xylene) ranged from 5.5 to 7.9 Tg yr−1, 2 % to 46 % larger than the estimate of the a priori emission inventory (5.4 Tg yr−1). Three out of our four inversion experiments indicated that the seasonal variation in Chinese NMVOC emissions was significantly stronger than indicated in the a priori inventory. Model simulations driven by the average of our top-down NMVOC emission estimates (which had a stronger seasonal variation than the a priori) showed that surface afternoon ozone concentrations over eastern China increased by 1–8 ppb in June and decreased by 1–10 ppb in December relative to the simulations using the a priori emissions and were in better agreement with measurements. We concluded that the satellite observations of formaldehyde and glyoxal together provided quantitative constraints on the emissions and source types of NMVOCs over China and improved our understanding on regional chemistry.


2018 ◽  
Author(s):  
Hansen Cao ◽  
Tzung-May Fu ◽  
Lin Zhang ◽  
Daven K. Henze ◽  
Christopher Chan Miller ◽  
...  

Abstract. We used the GEOS-Chem model and its adjoint to quantify Chinese non-methane volatile organic compound (NMVOC) emissions for the year 2007, using the vertical column concentrations of formaldehyde and glyoxal observed by the Global Ozone Monitoring Experiment-2A (GOME-2A) instrument and the Ozone Monitoring Instrument (OMI) as constraints. We conducted a series of inversion experiments using different combinations of satellite observations to explore the impacts on top-down emission estimates due to different satellite retrievals. Our top-down estimates for Chinese annual total NMVOC emission was 23.4 to 35.4 (average 30.8) Tg C y−1, including 13.5 to 19.7 (average 17.0) Tg C y−1 from anthropogenic sources, 8.9 to 14.8 (average 12.6) Tg C y−1 from biogenic sources, and 1.1 to 1.5 (average 1.2) Tg C y−1 from biomass burning. In comparison, the most widely-used bottom-up estimate for Chinese annual total NMVOC emission was 27.4 Tg C y−1, including 15.5 Tg C y−1 from anthropogenic sources, 10.8 Tg C y−1 from biogenic sources, and 1.1 Tg C y−1 from biomass burning. The simultaneous use of glyoxal and formaldehyde observations helped distinguish the NMVOC species from different sources and was essential in constraining anthropogenic emissions. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. Our top-down estimates for the Chinese annual emission of anthropogenic aromatics (benzene, toluene, and xylene) ranged from 5.0 to 7.3 Tg C y−1, 2 % to 49 % larger than the estimate of the bottom-up inventory (4.9 Tg C y−1). Model simulations using the average of our top-down NMVOC emission estimates showed that surface afternoon ozone concentrations over northern and central China increased 5–12 ppb in June and decreased 5–13 ppb in December relative to the simulations using the a priori emissions and were in better agreement with measurements. We concluded that the satellite observations of glyoxal and formaldehyde together provided quantitative constraints on the emissions and source types of NMVOCs over China and improved our understanding on regional chemistry.


2020 ◽  
Author(s):  
Can Li ◽  
Nickolay A. Krotkov ◽  
Peter J. T. Leonard ◽  
Simon Carn ◽  
Joanna Joiner ◽  
...  

Abstract. The Ozone Monitoring Instrument (OMI) has been providing global observations of SO2 pollution since 2004. Here we introduce the new anthropogenic SO2 vertical column density (VCD) dataset in the version 2 OMI SO2 product (OMSO2 V2). As with the previous version (OMSO2 V1.3), the new dataset is generated with an algorithm based on principal component analysis of OMI radiances, but features several updates. The most important among those is the use of expanded lookup tables and model a priori profiles to estimate SO2 Jacobians for individual OMI pixels, in order to better characterize pixel-to-pixel variations in SO2 sensitivity, including over snow and ice. Additionally, new data screening and spectral fitting schemes have been implemented to improve the quality of the spectral fit. As compared with the planetary boundary layer SO2 dataset in OMSO2 V1.3, the new dataset has substantially better data quality, especially over areas that are relatively clean or affected by the south Atlantic anomaly. The updated retrievals over snow/ice yield more realistic seasonal changes in SO2 at high latitudes and offer enhanced sensitivity to sources during wintertime. An error analysis has been conducted to assess uncertainties in SO2 VCDs from both the spectral fit and Jacobian calculations. The uncertainties from spectral fitting are reflected in SO2 slant column densities (SCDs) and largely depend on the signal-to-noise ratio of the measured radiances, as implied by the generally smaller SCD uncertainties over clouds or for lower solar zenith angles. The SCD uncertainties for individual pixels are estimated to be ~ 0.15–0.3 DU (Dobson Units) between ~ 40° S and ~ 40° N and to be ~ 0.2–0.5 DU at higher latitudes. The uncertainties from the Jacobians are approximately ~ 50–100 % over polluted areas, and primarily attributed to errors in SO2 a priori profiles and cloud pressures, as well as the lack of explicit treatment for aerosols. Finally, the daily mean and median SCDs over the presumably SO2-free equatorial East Pacific have increased by only ~ 0.0035 DU and ~ 0.003 DU respectively over the entire 15-year OMI record; while the standard deviation of SCDs has grown by only ~ 0.02 DU or ~ 10 %. Such remarkable long-term stability makes the new dataset particularly suitable for detecting regional changes in SO2 pollution.


2021 ◽  
Author(s):  
Richard J. Pope ◽  
Rebecca Kelly ◽  
Eloise A. Marais ◽  
Ailish M. Graham ◽  
Chris Wilson ◽  
...  

Abstract. Nitrogen oxides (NOx, NO+NO2) are potent air pollutants which directly impact on human health and which aid the formation of other hazardous pollutants such as ozone (O3) and particulate matter. In this study, we use satellite tropospheric column nitrogen dioxide (TCNO2) data to evaluate the spatiotemporal variability and magnitude of the United Kingdom (UK) bottom-up National Atmospheric Emissions Inventory (NAEI) NOx emissions. Although emissions and TCNO2 represent different quantities, for UK city sources we find a spatial correlation of ~0.5 between the NAEI NOx emissions and TCNO2 from the high-spatial-resolution TROPOspheric Monitoring Instrument (TROPOMI), suggesting a good spatial distribution of emission sources in the inventory. Between 2005 and 2015, the NAEI total UK NOx emissions and long-term TCNO2 record from the Ozone Monitoring Instrument (OMI), averaged over England, show decreasing trends of 4.4 % and 2.2 %, respectively. Top-down NOx emissions were derived in this study by applying a simple mass balance approach to TROPOMI observed downwind NO2 plumes from city sources. Overall, these top-down estimates were consistent with the NAEI, but for larger cities such as London and Manchester the inventory is significantly (> 25 %) less than the top-down emissions. This NAEI NOx emission underestimate is supported by comparing simulations from the GEOS-Chem atmospheric chemistry model, driven by the NAEI emissions, with satellite and surface NO2 observations over the UK. This yields substantial model negative biases, providing further evidence to demonstrate that the NAEI may be underestimating NOx emissions in London and Manchester.


2019 ◽  
Vol 12 (9) ◽  
pp. 4745-4778 ◽  
Author(s):  
Kai Yang ◽  
Xiong Liu

Abstract. New ozone (O3) profile climatologies are created from the Modern-Era Retrospective Analysis for Research and Applications version 2 (MERRA-2) O3 record between 2005 and 2016, within the period of Aura Microwave Limb Sounder (MLS) and Aura Ozone Monitoring Instrument (OMI) assimilation. These two climatologies consist of monthly mean O3 profiles and the corresponding covariances dependent on the local solar time, longitude (15∘), and latitude (10∘), which are parameterized by tropopause pressure and total O3 column. They are validated through comparisons, which show good agreements with previous O3 profile climatologies. Compared to a monthly zonal mean climatology, both tropopause- and column-dependent climatologies provide improved a priori information for profile and total O3 retrievals from remote sensing measurements. Furthermore, parameterization of the O3 profile with total column O3 usually reduces the natural variability of the resulting climatological profile in the upper stratosphere further than the tropopause parameterization, which usually performs better in the upper troposphere and lower stratosphere (UTLS). Therefore tropopause-dependent climatology is more appropriate for profile O3 retrieval for complementing the vertical resolution of backscattered ultraviolet (UV) spectra, while the column-dependent climatology is more suited for use in total O3 retrieval algorithms, with an advantage of complete profile specification without requiring ancillary information. Compared to previous column-dependent climatologies, the new MERRA-2 column-dependent climatology better captures the diurnal, seasonal, and spatial variations and dynamical changes in O3 profiles with higher resolutions in O3, latitude, longitude, and season. The new MERRA-2 climatologies contain the first quantitative characterization of O3 profile covariances, which facilitate a new approach to improve O3 profiles using the most probable patterns of profile adjustments represented by the empirical orthogonal functions (EOFs) of the covariance matrices. The MERRA-2 daytime column-dependent climatology is used in the combo O3 and SO2 algorithm for retrieval from the Earth Polychromatic Imaging Camera (EPIC) on board the Deep Space Climate Observatory (DSCOVR) satellite, the Ozone Mapping and Profiler Suite Nadir Mapper (OMPS-NM) on the Suomi National Polar Partnership (SNPP), and the Ozone Monitoring Instrument (OMI) on the Aura spacecraft.


2015 ◽  
Vol 15 (18) ◽  
pp. 10367-10383 ◽  
Author(s):  
Z. Lu ◽  
D. G. Streets ◽  
B. de Foy ◽  
L. N. Lamsal ◽  
B. N. Duncan ◽  
...  

Abstract. Satellite remote sensing of tropospheric nitrogen dioxide (NO2) can provide valuable information for estimating surface nitrogen oxides (NOx) emissions. Using an exponentially modified Gaussian (EMG) method and taking into account the effect of wind on observed NO2 distributions, we estimate 3-year moving-average emissions of summertime NOx from 35 US (United States) urban areas directly from NO2 retrievals of the Ozone Monitoring Instrument (OMI) during 2005–2014. Following conclusions of previous studies that the EMG method provides robust and accurate emission estimates under strong-wind conditions, we derive top-down NOx emissions from each urban area by applying the EMG method to OMI data with wind speeds greater than 3–5 m s−1. Meanwhile, we find that OMI NO2 observations under weak-wind conditions (i.e., < 3 m s−1) are qualitatively better correlated to the surface NOx source strength in comparison to all-wind OMI maps; therefore, we use them to calculate the satellite-observed NO2 burdens of urban areas and compare with NOx emission estimates. The EMG results show that OMI-derived NOx emissions are highly correlated (R > 0.93) with weak-wind OMI NO2 burdens as well as with bottom-up NOx emission estimates over 35 urban areas, implying a linear response of the OMI observations to surface emissions under weak-wind conditions. The simultaneous EMG-obtained effective NO2 lifetimes (~ 3.5 ± 1.3 h), however, are biased low in comparison to the summertime NO2 chemical lifetimes. In general, isolated urban areas with NOx emission intensities greater than ~ 2 Mg h−1 produce statistically significant weak-wind signals in 3-year average OMI data. From 2005 to 2014, we estimate that total OMI-derived NOx emissions over all selected US urban areas decreased by 49 %, consistent with reductions of 43, 47, 49, and 44 % in the total bottom-up NOx emissions, the sum of weak-wind OMI NO2 columns, the total weak-wind OMI NO2 burdens, and the averaged NO2 concentrations, respectively, reflecting the success of NOx control programs for both mobile sources and power plants. The decrease rates of these NOx-related quantities are found to be faster (i.e., −6.8 to −9.3 % yr−1) before 2010 and slower (i.e., −3.4 to −4.9 % yr−1) after 2010. For individual urban areas, we calculate the R values of pair-wise trends among the OMI-derived and bottom-up NOx emissions, the weak-wind OMI NO2 burdens, and ground-based NO2 measurements, and high correlations are found for all urban areas (median R= 0.8), particularly large ones (R up to 0.97). The results of the current work indicate that using the EMG method and considering the wind effect, the OMI data allow for the estimation of NOx emissions from urban areas and the direct constraint of emission trends with reasonable accuracy.


2020 ◽  
Vol 13 (11) ◽  
pp. 6175-6191
Author(s):  
Can Li ◽  
Nickolay A. Krotkov ◽  
Peter J. T. Leonard ◽  
Simon Carn ◽  
Joanna Joiner ◽  
...  

Abstract. The Ozone Monitoring Instrument (OMI) has been providing global observations of SO2 pollution since 2004. Here we introduce the new anthropogenic SO2 vertical column density (VCD) dataset in the version 2 OMI SO2 product (OMSO2 V2). As with the previous version (OMSO2 V1.3), the new dataset is generated with an algorithm based on principal component analysis of OMI radiances but features several updates. The most important among those is the use of expanded lookup tables and model a priori profiles to estimate SO2 Jacobians for individual OMI pixels, in order to better characterize pixel-to-pixel variations in SO2 sensitivity including over snow and ice. Additionally, new data screening and spectral fitting schemes have been implemented to improve the quality of the spectral fit. As compared with the planetary boundary layer SO2 dataset in OMSO2 V1.3, the new dataset has substantially better data quality, especially over areas that are relatively clean or affected by the South Atlantic Anomaly. The updated retrievals over snow/ice yield more realistic seasonal changes in SO2 at high latitudes and offer enhanced sensitivity to sources during wintertime. An error analysis has been conducted to assess uncertainties in SO2 VCDs from both the spectral fit and Jacobian calculations. The uncertainties from spectral fitting are reflected in SO2 slant column densities (SCDs) and largely depend on the signal-to-noise ratio of the measured radiances, as implied by the generally smaller SCD uncertainties over clouds or for smaller solar zenith angles. The SCD uncertainties for individual pixels are estimated to be ∼ 0.15–0.3 DU (Dobson units) between ∼ 40∘ S and ∼ 40∘ N and to be ∼ 0.2–0.5 DU at higher latitudes. The uncertainties from the Jacobians are approximately ∼ 50 %–100 % over polluted areas and are primarily attributed to errors in SO2 a priori profiles and cloud pressures, as well as the lack of explicit treatment for aerosols. Finally, the daily mean and median SCDs over the presumably SO2-free equatorial east Pacific have increased by only ∼ 0.0035 DU and ∼ 0.003 DU respectively over the entire 15-year OMI record, while the standard deviation of SCDs has grown by only ∼ 0.02 DU or ∼ 10%. Such remarkable long-term stability makes the new dataset particularly suitable for detecting regional changes in SO2 pollution.


2015 ◽  
Vol 15 (20) ◽  
pp. 11861-11884 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
M. Bauwens ◽  
I. De Smedt ◽  
M. Van Roozendael ◽  
...  

Abstract. The vertical columns of formaldehyde (HCHO) retrieved from two satellite instruments, the Global Ozone Monitoring Instrument-2 (GOME-2) on Metop-A and the Ozone Monitoring Instrument (OMI) on Aura, are used to constrain global emissions of HCHO precursors from open fires, vegetation and human activities in the year 2010. To this end, the emissions are varied and optimized using the adjoint model technique in the IMAGESv2 global CTM (chemical transport model) on a monthly basis and at the model resolution. Given the different local overpass times of GOME-2 (09:30 LT) and OMI (13:30 LT), the simulated diurnal cycle of HCHO columns is investigated and evaluated against ground-based optical measurements at seven sites in Europe, China and Africa. The modeled diurnal cycle exhibits large variability, reflecting competition between photochemistry and emission variations, with noon or early afternoon maxima at remote locations (oceans) and in regions dominated by anthropogenic emissions, late afternoon or evening maxima over fire scenes, and midday minima in isoprene-rich regions. The agreement between simulated and ground-based columns is generally better in summer (with a clear afternoon maximum at mid-latitude sites) than in winter, and the annually averaged ratio of afternoon to morning columns is slightly higher in the model (1.126) than in the ground-based measurements (1.043). The anthropogenic VOC (volatile organic compound) sources are found to be weakly constrained by the inversions on the global scale, mainly owing to their generally minor contribution to the HCHO columns, except over strongly polluted regions, like China. The OMI-based inversion yields total flux estimates over China close to the bottom-up inventory (24.6 vs. 25.5 TgVOC yr−1 in the a priori) with, however, pronounced increases in the northeast of China and reductions in the south. Lower fluxes are estimated based on GOME-2 HCHO columns (20.6 TgVOC yr−1), in particular over the northeast, likely reflecting mismatches between the observed and the modeled diurnal cycle in this region. The resulting biogenic and pyrogenic flux estimates from both optimizations generally show a good degree of consistency. A reduction of the global annual biogenic emissions of isoprene is derived, of 9 and 13 % according to GOME-2 and OMI, respectively, compared to the a priori estimate of 363 Tg in 2010. The reduction is largest (up to 25–40 %) in the Southeastern US, in accordance with earlier studies. The GOME-2 and OMI satellite columns suggest a global pyrogenic flux decrease by 36 and 33 %, respectively, compared to the GFEDv3 (Global Fire Emissions Database) inventory. This decrease is especially pronounced over tropical forests, such as in Amazonia, Thailand and Myanmar, and is supported by comparisons with CO observations from IASI (Infrared Atmospheric Sounding Interferometer). In contrast to these flux reductions, the emissions due to harvest waste burning are strongly enhanced over the northeastern China plain in June (by ca. 70 % in June according to OMI) as well as over Indochina in March. Sensitivity inversions showed robustness of the inferred estimates, which were found to lie within 7 % of the standard inversion results at the global scale.


2015 ◽  
Vol 8 (12) ◽  
pp. 13471-13524 ◽  
Author(s):  
R. Lutz ◽  
D. Loyola ◽  
S. Gimeno García ◽  
F. Romahn

Abstract. This paper describes an approach for cloud parameter retrieval (radiometric cloud fraction estimation) using the polarization measurements of the Global Ozone Monitoring Experiment-2 (GOME-2) on-board the MetOp-A/B satellites. The core component of the Optical Cloud Recognition Algorithm (OCRA) is the calculation of monthly cloud-free reflectances for a global grid (resolution of 0.2° in longitude and 0.2° in latitude) and to derive radiometric cloud fractions. These cloud fractions will serve as a priori information for the retrieval of cloud top height (CTH), cloud top pressure (CTP), cloud top albedo (CTA) and cloud optical thickness (COT) with the Retrieval Of Cloud Information using Neural Networks (ROCINN) algorithm. This approach is already being implemented operationally for the GOME/ERS-2 and SCIAMACHY/ENVISAT sensors and here we present version 3.0 of the OCRA algorithm applied to the GOME-2 sensors. Based on more than six years of GOME-2A data (February 2007–June 2013), reflectances are calculated for &amp;approx; 35 000 orbits. For each measurement a degradation correction as well as a viewing angle dependent and latitude dependent correction is applied. In addition, an empirical correction scheme is introduced in order to remove the effect of oceanic sun glint. A comparison of the GOME-2A/B OCRA cloud fractions with co-located AVHRR geometrical cloud fractions shows a general good agreement with a mean difference of −0.15±0.20. From operational point of view, an advantage of the OCRA algorithm is its extremely fast computational time and its straightforward transferability to similar sensors like OMI (Ozone Monitoring Instrument), TROPOMI (TROPOspheric Monitoring Instrument) on Sentinel 5 Precursor, as well as Sentinel 4 and Sentinel 5. In conclusion, it is shown that a robust, accurate and fast radiometric cloud fraction estimation for GOME-2 can be achieved with OCRA by using the polarization measurement devices (PMDs).


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