A 3D chemistry transport model study of changes in atmospheric ozone due to aircraft NOx emissions

1997 ◽  
Vol 31 (12) ◽  
pp. 1819-1836 ◽  
Author(s):  
W.M.F. Wauben ◽  
P.F.J.Van Velthoven ◽  
H. Kelder
Sensors ◽  
2018 ◽  
Vol 18 (9) ◽  
pp. 2893 ◽  
Author(s):  
Willem W. Verstraeten ◽  
Klaas Folkert Boersma ◽  
John Douros ◽  
Jason E. Williams ◽  
Henk Eskes ◽  
...  

Top-down estimates of surface NOX emissions were derived for 23 European cities based on the downwind plume decay of tropospheric nitrogen dioxide (NO2) columns from the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) chemistry transport model (CTM) and from Ozone Monitoring Instrument (OMI) satellite retrievals, averaged for the summertime period (April–September) during 2013. Here we show that the top-down NOX emissions derived from LOTOS-EUROS for European urban areas agree well with the bottom-up NOX emissions from the MACC-III inventory data (R2 = 0.88) driving the CTM demonstrating the potential of this method. OMI top-down NOX emissions over the 23 European cities are generally lower compared with the MACC-III emissions and their correlation is slightly lower (R2 = 0.79). The uncertainty on the derived NO2 lifetimes and NOX emissions are on average ~55% for OMI and ~63% for LOTOS-EUROS data. The downwind NO2 plume method applied on both LOTOS-EUROS and OMI tropospheric NO2 columns allows to estimate NOX emissions from urban areas, demonstrating that this is a useful method for real-time updates of urban NOX emissions with reasonable accuracy.


2007 ◽  
Vol 7 (1) ◽  
pp. 1143-1181 ◽  
Author(s):  
J. Damski ◽  
L. Thölix ◽  
L. Backman ◽  
J. Kaurola ◽  
P. Taalas ◽  
...  

Abstract. A Global 40-year simulation from 1980 to 2019 was performed with the FinROSE chemistry-transport model based on the use of coupled chemistry GCM-data. The main focus of our analysis is on climatological-scale processes in high latitudes. The resulting trend estimates for the past period (1980–1999) agree well with observation-based trend estimates. The results for the future period (2000–2019) suggest that the extent of seasonal ozone depletion over both northern and southern high-latitudes has likely reached its maximum. Furthermore, while climate change is expected to cool the stratosphere, this cooling is unlikely to accelerate significantly high latitude ozone depletion. However, the recovery of seasonal high latitude ozone losses will not take place during the next 15 years.


2003 ◽  
Vol 3 (1) ◽  
pp. 551-596 ◽  
Author(s):  
D. S. Stevenson ◽  
C. E. Johnson ◽  
E. J. Highwood ◽  
V. Gauci ◽  
W. J. Collins ◽  
...  

Abstract. Results from the first chemistry-transport model study of the impact of the 1783–1784 Laki fissure eruption (Iceland: 64° N, 17° W) upon atmospheric composition are presented. The eruption released an estimated 122 Tg(SO2) into the troposphere and lower stratosphere. The model has a high resolution tropopause region, and detailed sulphur chemistry. The simulated SO2 plume spreads over much of the Northern Hemisphere, polewards of ~40° N. About 70% of the SO2 gas is directly deposited to the surface before it can be oxidised to sulphuric acid aerosol. The main SO2 oxidants, OH and H2O2 , are depleted by up to 40% zonally, and the lifetime of SO2 consequently in-creases. Zonally averaged tropospheric SO2 concentrations over the first three months of the eruption exceed 20 ppbv, and sulphuric acid aerosol reaches ~2 ppbv. A total aerosol yield of 51–66 Tg(H2SO4 ) is produced. The mean aerosol lifetime is only 6–9 days, and the peak aerosol loading of the atmosphere is only ~7 Tg(H2SO4.2H2O). Due to the relatively short atmospheric residence times of both the SO2 and sulphate, the aerosol loading approximately mirrors the temporal evolution of emissions associated with the eruption. The model produces a reasonable simulation of the acid deposition found in Greenland ice cores. These results appear to be relatively insensitive to the vertical profile of emissions assumed, although if more of the emissions reached higher levels (>12 km), this would give longer lifetimes and larger aerosol yields. This study suggests that most previous estimates of the global aerosol loading associated with Laki have been generally too large in magnitude, and too long-lived. Environmental effects following the Laki eruption may have been dominated by the widespread deposition of SO2 gas rather than sulphuric acid aerosol.


2012 ◽  
Vol 12 (5) ◽  
pp. 2357-2380 ◽  
Author(s):  
Q. Tang ◽  
M. J. Prather

Abstract. We examine whether the individual ozone (O3) measurements from the four Aura instruments can quantify the stratosphere-troposphere exchange (STE) flux of O3, an important term of the tropospheric O3 budget. The level 2 (L2) Aura swath data and the nearly coincident ozone sondes for the years 2005–2006 are compared with the 4-D, high-resolution (1° × 1° × 40-layer × 0.5 h) model simulation of atmospheric ozone for the same period from the University of California, Irvine chemistry transport model (CTM). The CTM becomes a transfer standard for comparing individual profiles from these five, not-quite-coincident measurements of atmospheric ozone. Even with obvious model discrepancies identified here, the CTM can readily quantify instrument-instrument biases in the tropical upper troposphere and mid-latitude lower stratosphere. In terms of STE processes, all four Aura datasets have some skill in identifying stratosphere-troposphere folds, and we find several cases where both model and measurements see evidence of high-O3 stratospheric air entering the troposphere. In many cases identified in the model, however, the individual Aura profile retrievals in the upper troposphere and lower stratosphere show too much noise, as expected from their low sensitivity and coarse vertical resolution at and below the tropopause. These model-measurement comparisons of individual profiles do provide some level of confidence in the model-derived STE O3 flux, but it will be difficult to integrate this flux from the satellite data alone.


2014 ◽  
Vol 14 (21) ◽  
pp. 29237-29304 ◽  
Author(s):  
H. Petetin ◽  
M. Beekmann ◽  
A. Colomb ◽  
H. A. C. Denier van der Gon ◽  
J.-C. Dupont ◽  
...  

Abstract. High uncertainties affect black carbon (BC) emissions and, despite its important impact on air pollution and climate, very few BC emissions evaluations are found in the literature. This paper presents a novel approach, based on airborne measurements across the Paris plume, developed in order to evaluate BC and NOx emissions at the scale of a whole agglomeration. The methodology consists in integrating, for each transect, across the plume observed and simulated concentrations above background. This allows minimizing several error sources in the model (e.g. representativeness, chemistry, plume lateral dispersion). The procedure is applied with the CHIMERE chemistry-transport model to three inventories – the EMEP inventory, and the so-called TNO and TNO-MP inventories – over the month of July 2009. Various systematic uncertainty sources both in the model (e.g. boundary layer height, vertical mixing, deposition) and in observations (e.g. BC nature) are discussed and quantified, notably though sensitivity tests. A statistically significant (but moderate) overestimation is obtained on the TNO BC emissions and on EMEP and TNO-MP NOx emissions, as well as on the BC/NOx emission ratio in TNO-MP. The benefit of the airborne approach is discussed through a comparison with the BC/NOx ratio at a ground site in Paris, which additionally suggests potential error compensations in the BC emissions spatial distribution over the agglomeration.


2007 ◽  
Vol 7 (9) ◽  
pp. 2165-2181 ◽  
Author(s):  
J. Damski ◽  
L. Thölix ◽  
L. Backman ◽  
J. Kaurola ◽  
P. Taalas ◽  
...  

Abstract. A global 40-year simulation from 1980 to 2019 was performed with the FinROSE chemistry-transport model based on the use of coupled chemistry GCM-data. The main focus of our analysis is on climatological-scale processes in high latitudes. The resulting trend estimates for the past period (1980–1999) agree well with observation-based trend estimates. The results for the future period (2000–2019) suggest that the extent of seasonal ozone depletion over both northern and southern high-latitudes has likely reached its maximum. Furthermore, while climate change is expected to cool the stratosphere, this cooling is unlikely to accelerate significantly high latitude ozone depletion. However, the recovery of seasonal high latitude ozone losses will not take place during the next 15 years.


2010 ◽  
Vol 10 (3) ◽  
pp. 1345-1359 ◽  
Author(s):  
G. G. Pfister ◽  
L. K. Emmons ◽  
D. P. Edwards ◽  
A. Arellano ◽  
T. Campos ◽  
...  

Abstract. We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part B) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and dynamics from changes in source strength. Interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 1/3 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 2/3 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.


Atmosphere ◽  
2021 ◽  
Vol 12 (2) ◽  
pp. 192
Author(s):  
Rita Cesari ◽  
Tony Christian Landi ◽  
Massimo D’Isidoro ◽  
Mihaela Mircea ◽  
Felicita Russo ◽  
...  

This work presents the on-line coupled meteorology–chemistry transport model BOLCHEM, based on the hydrostatic meteorological BOLAM model, the gas chemistry module SAPRC90, and the aerosol dynamic module AERO3. It includes parameterizations to describe natural source emissions, dry and wet removal processes, as well as the transport and dispersion of air pollutants. The equations for different processes are solved on the same grid during the same integration step, by means of a time-split scheme. This paper describes the model and its performance at horizontal resolution of 0.2∘× 0.2∘ over Europe and 0.1∘× 0.1∘ in a nested configuration over Italy, for one year run (December 2009–November 2010). The model has been evaluated against the AIRBASE data of the European Environmental Agency. The basic statistics for higher resolution simulations of O3, NO2 and particulate matter concentrations (PM2.5 and PM10) have been compared with those from Copernicus Atmosphere Monitoring Service (CAMS) ensemble median. In summer, for O3 we found a correlation coefficient R of 0.72 and mean bias of 2.15 over European domain and a correlation coefficient R of 0.67 and mean bias of 2.36 over Italian domain. PM10 and PM2.5 are better reproduced in the winter, the latter with a correlation coefficient R of 0.66 and the mean bias MB of 0.35 over Italian domain.


Atmosphere ◽  
2021 ◽  
Vol 12 (7) ◽  
pp. 900
Author(s):  
Ioanna Skoulidou ◽  
Maria-Elissavet Koukouli ◽  
Arjo Segers ◽  
Astrid Manders ◽  
Dimitris Balis ◽  
...  

In this work, we investigate the ability of a data assimilation technique and space-borne observations to quantify and monitor changes in nitrogen oxides (NOx) emissions over Northwestern Greece for the summers of 2018 and 2019. In this region, four lignite-burning power plants are located. The data assimilation technique, based on the Ensemble Kalman Filter method, is employed to combine space-borne atmospheric observations from the high spatial resolution Sentinel-5 Precursor (S5P) Tropospheric Monitoring Instrument (TROPOMI) and simulations using the LOTOS-EUROS Chemical Transport model. The Copernicus Atmosphere Monitoring Service-Regional European emissions (CAMS-REG, version 4.2) inventory based on the year 2015 is used as the a priori emissions in the simulations. Surface measurements of nitrogen dioxide (NO2) from air quality stations operating in the region are compared with the model surface NO2 output using either the a priori (base run) or the a posteriori (assimilated run) NOx emissions. Relative to the a priori emissions, the assimilation suggests a strong decrease in concentrations for the station located near the largest power plant, by 80% in 2019 and by 67% in 2018. Concerning the estimated annual a posteriori NOx emissions, it was found that, for the pixels hosting the two largest power plants, the assimilated run results in emissions decreased by ~40–50% for 2018 compared to 2015, whereas a larger decrease, of ~70% for both power plants, was found for 2019, after assimilating the space-born observations. For the same power plants, the European Pollutant Release and Transfer Register (E-PRTR) reports decreased emissions in 2018 and 2019 compared to 2015 (−35% and −38% in 2018, −62% and −72% in 2019), in good agreement with the estimated emissions. We further compare the a posteriori emissions to the reported energy production of the power plants during the summer of 2018 and 2019. Mean decreases of about −35% and−63% in NOx emissions are estimated for the two larger power plants in summer of 2018 and 2019, respectively, which are supported by similar decreases in the reported energy production of the power plants (~−30% and −70%, respectively).


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