scholarly journals Evaluating BC and NO<sub>x</sub> emission inventories for the Paris region from MEGAPOLI aircraft measurements

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 ◽  
...  
Keyword(s):  
Transport Model ◽  
Vertical Mixing ◽  
Nox Emissions ◽  
Error Sources ◽  
Chemistry Transport Model ◽  
Airborne Measurements ◽  
Boundary Layer Height ◽  
Uncertainty Sources ◽  
Novel Approach ◽  
Sensitivity Tests

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.

scholarly journals Evaluating BC and NO<sub><i>x</i></sub> emission inventories for the Paris region from MEGAPOLI aircraft measurements

2015 ◽  
Vol 15 (17) ◽  
pp. 9799-9818 ◽  
Author(s):  
H. Petetin ◽  
M. Beekmann ◽  
A. Colomb ◽  
H. A. C. Denier van der Gon ◽  
J.-C. Dupont ◽  
...  
Keyword(s):  
Transport Model ◽  
Vertical Mixing ◽  
Nox Emissions ◽  
Emission Inventories ◽  
Error Sources ◽  
Airborne Measurements ◽  
Boundary Layer Height ◽  
Uncertainty Sources ◽  
Novel Approach ◽  
Sensitivity Tests

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, France, 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 for several error sources (e.g., representativeness, chemistry, plume lateral dispersion) to be minimized in the model used. 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 through sensitivity tests. Large uncertainty values are determined in our results, which limits the usefulness of the method to rather strongly erroneous emission inventories. A statistically significant (but moderate) overestimation is obtained for the TNO BC emissions and the EMEP and TNO-MP NOx emissions, as well as for 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 a spatially heterogeneous error in BC emissions over the agglomeration.

scholarly journals Top-Down NOX Emissions of European Cities Based on the Downwind Plume of Modelled and Space-Borne Tropospheric NO2 Columns

Sensors ◽  
2018 ◽  
Vol 18 (9) ◽  
pp. 2893 ◽  
Author(s):  
Willem W. Verstraeten ◽  
Klaas Folkert Boersma ◽  
John Douros ◽  
Jason E. Williams ◽  
Henk Eskes ◽  
...  
Keyword(s):  
Urban Areas ◽  
Transport Model ◽  
Nox Emissions ◽  
Inventory Data ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
Chemistry Transport Model ◽  
European Cities ◽  
Tropospheric No2

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.

scholarly journals The constraint of CO<sub>2</sub> measurements made onboard passenger aircraft on surface-atmosphere fluxes: the impact of transport model errors in vertical mixing

2016 ◽  
Author(s):  
Shreeya Verma ◽  
Julia Marshall ◽  
Christoph Gerbig ◽  
Christian Roedenbeck ◽  
Kai Uwe Totsche
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
Vertical Mixing ◽  
Synthetic Data ◽  
Vertical Profiles ◽  
Model Errors ◽  
Transport Models ◽  
Boundary Layer Height ◽  
Temporal Sampling ◽  
The Impact

Abstract. Inaccurate representation of atmospheric processes by transport models is a dominant source of uncertainty in inverse analyses and can lead to large discrepancies in the retrieved flux estimates. We investigate the impact of uncertainties in vertical transport as simulated by atmospheric transport models on fluxes retrieved using vertical profiles from aircraft as an observational constraint. Our numerical experiments are based on synthetic data with realistic spatial and temporal sampling of aircraft measurements. The impact of such uncertainties on the flux retrieved using the ground-based network with those retrieved using the aircraft profiles are compared. We find that the posterior flux retrieved using aircraft profiles is less susceptible to errors in boundary layer height as compared to the ground- based network. This highlights the benefit of utilizing atmospheric observations made onboard aircraft over surface measurements for flux estimation using inverse methods. We further use synthetic vertical profiles of CO2 in an inversion to estimate the potential of these measurements, which will be made available through the IAGOS (In-Service Aircraft for a Global Observing System) project in future, in constraining the regional carbon budget. Our results show that the regions tropical Africa and temperate Eurasia, that are under constrained by the existing surface based network, will benefit the most from these measurements, the reduction of posterior flux uncertainty being about 7 to 10 %.

scholarly journals Description and evaluation of a detailed gas-phase chemistry scheme in the TM5-MP global chemistry transport model (r112)

2020 ◽  
Author(s):  
Stelios Myriokefalitakis ◽  
Nikos Daskalakis ◽  
Angelos Gkouvousis ◽  
Andreas Hilboll ◽  
Twan van Noije ◽  
...  
Keyword(s):  
Gas Phase ◽  
Transport Model ◽  
Vertical Mixing ◽  
Three Dimensional ◽  
Chemical Mechanism ◽  
Aerosol Formation ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
Time Requirements ◽  
Phase Chemistry

Abstract. This work documents and evaluates the tropospheric gas-phase chemical mechanism MOGUNTIA in the three-dimensional chemistry transport model TM5-MP. Compared to the modified CB05 chemical mechanism previously used in the model, the MOGUNTIA includes a detailed representation of the light hydrocarbons (C1-C4) and isoprene, along with a simplified chemistry representation of terpenes and aromatics. Another feature implemented in TM5-MP for this work is the use of the Rosenbrock solver in the chemistry code, which can replace the classical Euler Backward Integration method of the model. Global budgets of ozone (O3), carbon monoxide (CO), hydroxyl radicals (OH), nitrogen oxides (NOX) and volatile organic compounds (VOCs) are here analyzed and their mixing ratios are compared with a series of surface, aircraft and satellite observations for the year 2006. Both mechanisms appear to be able to represent satisfactorily observed mixing ratios of important trace gases, with the MOGUNTIA chemistry configuration yielding lower biases compared to measurements in most of the cases. However, the two chemical mechanisms fail to reproduce the observed mixing ratios of light VOCs, indicating insufficient primary emission source strengths, too weak vertical mixing in the boundary layer, and/or a low bias in the secondary contribution of C2-C3 organics via VOC atmospheric oxidation. Relative computational memory and time requirements of the different model configurations are also compared and discussed. Overall, compared to other chemistry schemes in use in global CTMs, the MOGUNTIA scheme simulates a large suite of oxygenated VOCs that are observed in the atmosphere at significant levels and are involved in aerosol formation, expanding, thus, the applications of TM5-MP.

scholarly journals The climate impact of ship NO<sub>x</sub> emissions: an improved estimate accounting for plume chemistry

2014 ◽  
Vol 14 (3) ◽  
pp. 3427-3458
Author(s):  
C. D. Holmes ◽  
M. J. Prather ◽  
G. C. M. Vinken
Keyword(s):  
Radiative Forcing ◽  
Transport Model ◽  
Parametric Representation ◽  
Climate Impact ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Rf Components ◽  
Maritime Shipping ◽  
Sensitivity Tests ◽  
Emission Changes

Abstract. Nitrogen oxide (NOx) emissions from maritime shipping produce ozone (O3) and hydroxyl radicals (OH), which in turn destroy methane (CH4). The balance between this warming (due to O3) and cooling (due to CH4) determines the net effect of ship NOx on climate. Previous estimates of the chemical impact and radiative forcing (RF) of ship NOx have generally assumed that plumes of ship exhaust are instantly diluted into model grid cells spanning hundreds of kilometers, even though this is known to produce biased results. Here we improve the parametric representation of exhaust-gas chemistry developed in the GEOS-Chem chemical transport model (CTM) to provide the first estimate of RF from shipping that accounts for sub-grid-scale ship plume chemistry. The CTM now calculates O3 production and CH4 loss both within and outside the exhaust plumes and also accounts for the effect of wind speed. With the improved modeling of plumes, ship NOx perturbations are smaller than suggested by the ensemble of past global modeling studies, but if we assume instant dilution of ship NOx on the grid scale, the CTM reproduces previous model results. Our best estimates of the RF components from increasing ship NOx emissions by 1 Tg(N) yr−1 are smaller than given in the past literature: +3.4 ± 0.85 mW m−2 from the short-lived ozone increase, −5.0 ± 1.1 mW m−2 from the CH4 decrease, and −1.7 ± 0.7 mW m−2 from the long-lived O3 decrease that accompanies the CH4 change. The resulting net RF is −3.3 ± 1.8 mW m−2 for emissions of 1 Tg(N) yr−1. Due to non-linearity in O3 production as a function of background NOx, RF from large changes in ship NOx emissions, such as the increase since preindustrial times, is about 20% larger than this RF value for small marginal emission changes. Using sensitivity tests in one CTM, we quantify sources of uncertainty in the RF components and causes of the ±30% spread in past model results. The main source of uncertainty is the composition of the background atmosphere in the CTM, which is driven by model formulation (±10 to 20%) and the plausible range of anthropogenic emissions (±10%).

scholarly journals Comprehensive evaluations of diurnal NO<sub>2</sub> measurements during DISCOVER-AQ 2011: effects of resolution-dependent representation of NO<sub><i>x</i></sub> emissions

2021 ◽  
Vol 21 (14) ◽  
pp. 11133-11160
Author(s):  
Jianfeng Li ◽  
Yuhang Wang ◽  
Ruixiong Zhang ◽  
Charles Smeltzer ◽  
Andrew Weinheimer ◽  
...  
Keyword(s):  
Transport Model ◽  
Global Radiation ◽  
Vertical Mixing ◽  
Spatial Variations ◽  
Radiation Budget ◽  
Nox Emissions ◽  
Ozone Monitoring Instrument ◽  
Vertical Column ◽  
Model Simulations ◽  
Ozone Monitoring

Abstract. Nitrogen oxides (NOx = NO + NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations in NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements and surface EPA Air Quality System (AQS) observations as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; GOME-2A: Global Ozone Monitoring Experiment – 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument in July 2011 during the DISCOVER-AQ campaign over the Baltimore–Washington region. The model simulations at 36 and 4 km resolutions are in reasonably good agreement with the regional mean temporospatial NO2 observations in the daytime. However, we find significant overestimations (underestimations) of model-simulated NO2 (O3) surface concentrations during nighttime, which can be mitigated by enhancing nocturnal vertical mixing in the model. Another discrepancy is that Pandora-measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. The higher-resolution 4 km simulations tend to show larger biases compared to the observations due largely to the larger spatial variations in NOx emissions in the model when the model spatial resolution is increased from 36 to 4 km. OMI, GOME-2A, and the high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than corresponding 36 and 4 km model simulations, likely reflecting the spatial distribution bias of NOx emissions in the National Emissions Inventory (NEI) 2011.

scholarly journals The constraint of CO<sub>2</sub> measurements made onboard passenger aircraft on surface–atmosphere fluxes: the impact of transport model errors in vertical mixing

2017 ◽  
Vol 17 (9) ◽  
pp. 5665-5675 ◽  
Author(s):  
Shreeya Verma ◽  
Julia Marshall ◽  
Christoph Gerbig ◽  
Christian Rödenbeck ◽  
Kai Uwe Totsche
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
Vertical Mixing ◽  
Synthetic Data ◽  
Vertical Profiles ◽  
Model Errors ◽  
Transport Models ◽  
Boundary Layer Height ◽  
Temporal Sampling ◽  
The Impact

Abstract. Inaccurate representation of atmospheric processes by transport models is a dominant source of uncertainty in inverse analyses and can lead to large discrepancies in the retrieved flux estimates. We investigate the impact of uncertainties in vertical transport as simulated by atmospheric transport models on fluxes retrieved using vertical profiles from aircraft as an observational constraint. Our numerical experiments are based on synthetic data with realistic spatial and temporal sampling of aircraft measurements. The impact of such uncertainties on the flux retrieved using the ground-based network and those retrieved using the aircraft profiles are compared. We find that the posterior flux retrieved using aircraft profiles is less susceptible to errors in boundary layer height, compared to the ground-based network. This finding highlights a benefit of utilizing atmospheric observations made onboard aircraft over surface measurements for flux estimation using inverse methods. We further use synthetic vertical profiles of CO2 in an inversion to estimate the potential of these measurements, which will be made available through the IAGOS (In-service Aircraft for a Global Observing System) project in the future, in constraining the regional carbon budget. Our results show that the regions of tropical Africa and temperate Eurasia, that are under-constrained by the existing surface-based network, will benefit the most from these measurements, with a reduction of posterior flux uncertainty of about 7 to 10 %.

Sign in / Sign up

Export Citation Format

Share Document