scholarly journals Impacts of global NO<sub><i>x</i></sub> inversions on NO<sub>2</sub> and ozone simulations

2020 ◽  
Vol 20 (21) ◽  
pp. 13109-13130 ◽  
Author(s):  
Zhen Qu ◽  
Daven K. Henze ◽  
Owen R. Cooper ◽  
Jessica L. Neu
Keyword(s):  
Western Europe ◽  
Surface Ozone ◽  
Remote Sensing Data ◽  
Global Scale ◽  
Diurnal Variations ◽  
Nox Emissions ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
The Us ◽  
Global Background

Abstract. Tropospheric NO2 and ozone simulations have large uncertainties, but their biases, seasonality, and trends can be improved with NO2 assimilations. We perform global top-down estimates of monthly NOx emissions using two Ozone Monitoring Instrument (OMI) NO2 retrievals (NASAv3 and DOMINOv2) from 2005 to 2016 through a hybrid 4D-Var/mass balance inversion. Discrepancy in NO2 retrieval products is a major source of uncertainties in the top-down NOx emission estimates. The different vertical sensitivities in the two NO2 retrievals affect both magnitude and seasonal variations of top-down NOx emissions. The 12-year averages of regional NOx budgets from the NASA posterior emissions are 37 % to 53 % smaller than the DOMINO posterior emissions. Consequently, the DOMINO posterior surface NO2 simulations greatly reduced the negative biases in China (by 15 %) and the US (by 22 %) compared to surface NO2 measurements. Posterior NOx emissions show consistent trends over China, the US, India, and Mexico constrained by the two retrievals. Emission trends are less robust over South America, Australia, western Europe, and Africa, where the two retrievals show less consistency. NO2 trends have more consistent decreases (by 26 %) with the measurements (by 32 %) in the US from 2006 to 2016 when using the NASA posterior emissions. The performance of posterior ozone simulations has spatial heterogeneities from region to region. On a global scale, ozone simulations using NASA-based emissions alleviate the double peak in the prior simulation of global ozone seasonality. The higher abundances of NO2 from the DOMINO posterior simulations increase the global background ozone concentrations and therefore reduce the negative biases more than the NASA posterior simulations using GEOS-Chem v12 at remote sites. Compared to surface ozone measurements, posterior simulations have more consistent magnitude and interannual variations than the prior estimates, but the performance from the NASA-based and DOMINO-based emissions varies across ozone metrics. The limited availability of remote-sensing data and the use of prior NOx diurnal variations hinder improvement of ozone diurnal variations from the assimilation, and therefore have mixed performance on improving different ozone metrics. Additional improvements in posterior NO2 and ozone simulations require more precise and consistent NO2 retrieval products, more accurate diurnal variations of NOx and VOC emissions, and improved simulations of ozone chemistry and depositions.

scholarly journals Improving NO<sub>2</sub> and ozone simulations through global NO<sub><i>x</i></sub> emission inversions

2020 ◽  
Author(s):  
Zhen Qu ◽  
Daven K. Henze ◽  
Owen R. Cooper ◽  
Jessica L. Neu
Keyword(s):  
Tropospheric Ozone ◽  
Surface Ozone ◽  
Nox Emissions ◽  
Regional Models ◽  
Top Down ◽  
Double Peak ◽  
The Us ◽  
Ozone Trends ◽  
Remote Sites ◽  
Temporal Focus

Abstract. Tropospheric ozone simulations have large uncertainties, but their biases, seasonality and trends can be improved with more accurate estimates of precursor gas emissions. We perform global top-down estimates of monthly NOx emissions using two OMI NO2 retrievals (NASAv3 and DOMINOv2) from 2005 to 2016 through a hybrid 4D-Var/mass balance inversion. The 12-year averages of regional NOx budgets from the NASA posterior emissions are 37 % to 53 % smaller than the DOMINO posterior. Compared to surface NO2 measurements, GEOS-Chem adjoint NO2 simulations using the DOMINO posterior NOx emissions have smaller biases in China (by 15 %) and the US (by 22 %), but NO2 trends have more consistent decreases (by 26 %) with the measurements (by 32 %) in the US from 2006 to 2016 when using the NASA posterior. The two posterior NOx emissions datasets have different strengths with respect to simulation of ozone concentrations. Simulations using NASA-based emissions provide better agreement for polluted conditions. Ozone from these shows the highest correlation (R2 = 0.88) with annual MDA8 ozone trends and alleviates the double peak in the prior simulation of global ozone seasonality. The DOMINO-based emissions, on the other hand, are better for simulating ozone at remote sites, making them well-suited to generation of boundary conditions for regional models, and in capturing the interannual variability of daytime-average (R2 = 0.72–0.81) and 24-hour average (R2 = 0.88–0.96) surface ozone. We recommend using NOx emission datasets that have the best performance in the corresponding spatial domain and temporal focus to improve ozone simulations.

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 Modeling the regional impact of ship emissions on NO<sub>x</sub> and ozone levels over the Eastern Atlantic and Western Europe using ship plume parameterization

2010 ◽  
Vol 10 (14) ◽  
pp. 6645-6660 ◽  
Author(s):  
P. Huszar ◽  
D. Cariolle ◽  
R. Paoli ◽  
T. Halenka ◽  
M. Belda ◽  
...  
Keyword(s):  
Large Scale ◽  
Western Europe ◽  
Surface Ozone ◽  
Chemical Species ◽  
Nitrogen Monoxide ◽  
Ozone Production ◽  
Nox Emissions ◽  
Ship Emissions ◽  
Concentrated Source ◽  
The Impact

Abstract. In general, regional and global chemistry transport models apply instantaneous mixing of emissions into the model's finest resolved scale. In case of a concentrated source, this could result in erroneous calculation of the evolution of both primary and secondary chemical species. Several studies discussed this issue in connection with emissions from ships and aircraft. In this study, we present an approach to deal with the non-linear effects during dispersion of NOx emissions from ships. It represents an adaptation of the original approach developed for aircraft NOx emissions, which uses an exhaust tracer to trace the amount of the emitted species in the plume and applies an effective reaction rate for the ozone production/destruction during the plume's dilution into the background air. In accordance with previous studies examining the impact of international shipping on the composition of the troposphere, we found that the contribution of ship induced surface NOx to the total reaches 90% over remote ocean and makes 10–30% near coastal regions. Due to ship emissions, surface ozone increases by up to 4–6 ppbv making 10% contribution to the surface ozone budget. When applying the ship plume parameterization, we show that the large scale NOx decreases and the ship NOx contribution is reduced by up to 20–25%. A similar decrease was found in the case of O3. The plume parameterization suppressed the ship induced ozone production by 15–30% over large areas of the studied region. To evaluate the presented parameterization, nitrogen monoxide measurements over the English Channel were compared with modeled values and it was found that after activating the parameterization the model accuracy increases.

scholarly journals Ozone and NO<sub>x</sub> chemistry in the eastern US: evaluation of CMAQ/CB05 with satellite (OMI) data

2015 ◽  
Vol 15 (4) ◽  
pp. 4427-4461 ◽  
Author(s):  
T. P. Canty ◽  
L. Hembeck ◽  
T. P. Vinciguerra ◽  
D. C. Anderson ◽  
D. L. Goldberg ◽  
...  
Keyword(s):  
Air Quality ◽  
Surface Ozone ◽  
Quality Standards ◽  
Ambient Air ◽  
Daily Maximum ◽  
Air Quality Model ◽  
Ozone Monitoring Instrument ◽  
Air Quality Standards ◽  
The Us ◽  
Us Northeast

Abstract. Regulatory air quality models, such as the Community Multiscale Air Quality model (CMAQ), are used by federal and state agencies to guide policy decisions that determine how to best achieve adherence with National Ambient Air Quality Standards for surface ozone. We use observations of ozone and its important precursor NO2 to test the representation of the photochemistry and emission of ozone precursors within CMAQ. Observations of tropospheric column NO2 from the Ozone Monitoring Instrument (OMI), retrieved by two independent groups, show that the model overestimates urban NO2 and underestimates rural NO2 under all conditions examined for July and August 2011 in the US Northeast. The overestimate of the urban to rural ratio of tropospheric column NO2 for this baseline run of CMAQ (CB05 mechanism, mobile NOx emissions from the National Emissions Inventory; isoprene emissions from MEGAN v2.04) suggests this model may under estimate the importance of interstate transport of NOx. This CMAQ simulation leads to a considerable overestimate of the 2 month average of 8 h daily maximum surface ozone in the US Northeast, as well as an overestimate of 8 h ozone at AQS sites during days when the state of Maryland experienced NAAQS exceedances. We have implemented three changes within CMAQ motivated by OMI NO2 as well as aircraft observations obtained in July 2011 during the NASA DISCOVER-AQ campaign: (a) the modeled lifetime of organic nitrates within CB05 has been reduced by a factor of 10, (b) emissions of NOx from mobile sources has been reduced by a factor of 2, and (c) isoprene emissions have been reduced by using MEGAN v2.10 rather than v2.04. Compared to the baseline simulation, the CMAQ run using all three of these changes leads to a considerably better simulation of the ratio of urban to rural column NO2, better agreement with the 2 month average of daily 8 h maximum ozone in the US Northeast, fewer number of false positives of an ozone exceedance throughout the domain, as well as an unbiased simulation of surface ozone at ground based AQS sites in Maryland that experienced an ozone exceedance during July and August 2007. These modifications to CMAQ may provide a framework for use in studies focused on achieving future adherence to specific air quality standards for surface ozone by reducing emission of NOx from various anthropogenic sectors.

scholarly journals Exploiting satellite measurements to reduce uncertainties in UK bottom-up NO<sub>x</sub> emission estimates

2021 ◽  
Author(s):  
Richard J. Pope ◽  
Rebecca Kelly ◽  
Eloise A. Marais ◽  
Ailish M. Graham ◽  
Chris Wilson ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Spatiotemporal Variability ◽  
Nox Emissions ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
Bottom Up ◽  
Emissions Inventory ◽  
Monitoring Instrument ◽  
Hazardous Pollutants ◽  
The Uk

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.

scholarly journals Using satellite observations of tropospheric NO<sub>2</sub> columns to infer long-term trends in US NO<sub><i>x</i></sub> emissions: the importance of accounting for the free tropospheric NO<sub>2</sub> background

2019 ◽  
Vol 19 (13) ◽  
pp. 8863-8878 ◽  
Author(s):  
Rachel F. Silvern ◽  
Daniel J. Jacob ◽  
Loretta J. Mickley ◽  
Melissa P. Sulprizio ◽  
Katherine R. Travis ◽  
...  
Keyword(s):  
Environmental Protection Agency ◽  
Model Simulation ◽  
Satellite Observations ◽  
Nox Emissions ◽  
Ozone Monitoring Instrument ◽  
Relative Contribution ◽  
Steady Decrease ◽  
The Us ◽  
Tropospheric No2 ◽  
Long Term Trends

Abstract. The National Emission Inventory (NEI) of the US Environmental Protection Agency (EPA) reports a steady decrease in US NOx emissions over the 2005–2017 period at a rate of 0.1 Tg N a−1 (53 % decrease over the period), reflecting sustained efforts to improve air quality. Tropospheric NO2 columns observed by the satellite-based Ozone Monitoring Instrument (OMI) over the US show a steady decrease until 2009 but a flattening afterward, which has been attributed to a flattening of NOx emissions, contradicting the NEI. We show here that the steady 2005–2017 decrease in NOx emissions reported by the NEI is in fact largely consistent with observed network trends of surface NO2 and ozone concentrations. The OMI NO2 trend is instead similar to that observed for nitrate wet deposition fluxes, which is weaker than that for anthropogenic NOx emissions, due to a large and increasing relative contribution of non-anthropogenic background sources of NOx (mainly lightning and soils). This is confirmed by contrasting OMI NO2 trends in urban winter, where the background is low and OMI NO2 shows a 2005–2017 decrease consistent with the NEI, and rural summer, where the background is high and OMI NO2 shows no significant 2005–2017 trend. A GEOS-Chem model simulation driven by NEI emission trends for the 2005–2017 period reproduces these different trends, except for the post-2009 flattening of OMI NO2, which we attribute to a model underestimate of free tropospheric NO2. Better understanding is needed of the factors controlling free tropospheric NO2 in order to relate satellite observations of tropospheric NO2 columns to the underlying NOx emissions and their trends. Focusing on urban winter conditions in the satellite data minimizes the effect of this free tropospheric background.

scholarly journals Global-Scale Patterns and Trends in Tropospheric NO2 Concentrations, 2005–2018

2020 ◽  
Vol 12 (21) ◽  
pp. 3526 ◽  
Author(s):  
Sadegh Jamali ◽  
Daniel Klingmyr ◽  
Torbern Tagesson
Keyword(s):  
Western Europe ◽  
Temporal Trends ◽  
Global Scale ◽  
Air Pollutant ◽  
Ozone Monitoring Instrument ◽  
Substantial Impact ◽  
Tropospheric No2 ◽  
Eastern Usa ◽  
High Concentrations ◽  
Using Data

Nitrogen dioxide (NO2) is an important air pollutant with both environmental and epidemiological effects. The main aim of this study is to analyze spatial patterns and temporal trends in tropospheric NO2 concentrations globally using data from the satellite-based Ozone Monitoring Instrument (OMI). Additional aims are to compare the satellite data with ground-based observations, and to find the timing and magnitude of greatest breakpoints in tropospheric NO2 concentrations for the time period 2005–2018. The OMI NO2 concentrations showed strong relationships with the ground-based observations, and inter-annual patterns were especially well reproduced. Eastern USA, Western Europe, India, China and Japan were identified as hotspot areas with high concentrations of NO2. The global average trend indicated slightly increasing NO2 concentrations (0.004 × 1015 molecules cm−2 y−1) in 2005–2018. The contribution of different regions to this global trend showed substantial regional differences. Negative trends were observed for most of Eastern USA, Western Europe, Japan and for parts of China, whereas strong, positive trends were seen in India, parts of China and in the Middle East. The years 2005 and 2007 had the highest occurrence of negative breakpoints, but the trends thereafter in general reversed, and the highest tropospheric NO2 concentrations were observed for the years 2017–2018. This indicates that the anthropogenic contribution to air pollution is still a major issue and that further actions are necessary to reduce this contribution, having a substantial impact on human and environmental health.

scholarly journals Comparison and evaluation of anthropogenic emissions of SO<sub>2</sub> and NO<sub>x over China

2017 ◽  
Author(s):  
Meng Li ◽  
Zbigniew Klimont ◽  
Qiang Zhang ◽  
Randall V. Martin ◽  
Bo Zheng ◽  
...  
Keyword(s):  
Comprehensive Evaluation ◽  
Model Performance ◽  
Chemical Transport ◽  
Nox Emissions ◽  
Emission Inventories ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
Bottom Up ◽  
Essential Input ◽  
Inventory Development

Abstract. Bottom-up emission inventories provide primary understanding of sources of air pollution and essential input of chemical transport models. Focusing on SO2 and NOx, we conducted a comprehensive evaluation of two widely-used anthropogenic emission inventories over China, ECLIPSE and MIX, to explore the potential sources of uncertainties and find the clues in improving emission inventories. We first compared the activity rates and emission factors used in two inventories, and investigated the reasons of differences and the impacts on emission estimates. We found that SO2 emission estimates are consistent between two inventories (with 1 % differences), while NOx emissions in ECLIPSE's estimates are 16 % lower than those of MIX. Discrepancies at sectorial and provincial level are much higher. We then examined the impacts of different inventories on model performance, by using the nested GEOS-Chem model. We finally derived top-down NOx emissions by using the NO2 columns from the Ozone Monitoring Instrument (OMI) and compared with the bottom-up estimates. To our knowledge, this is the first work where source-sector comparisons are made along with the remote sensing retrievals and chemical transport modeling. Through the comparison between bottom-up emission inventories and evaluation with top-down information, we summarized the potential directions for further improvement in inventory development.

scholarly journals An Estimation of Top-Down NOx Emissions from OMI Sensor Over East Asia

2020 ◽  
Vol 12 (12) ◽  
pp. 2004 ◽  
Author(s):  
Kyung M. Han ◽  
Hyun S. Kim ◽  
Chul H. Song
Keyword(s):  
East Asia ◽  
Mass Conservation ◽  
Weather Research And Forecasting ◽  
Nox Emissions ◽  
Wind Vector ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
Model Simulations ◽  
Ozone Monitoring ◽  
Atmospheric Factors

This study focuses on the estimation of top-down NOx emissions over East Asia, integrating information on the levels of NO2 and NO, wind vector, and geolocation from Ozone Monitoring Instrument (OMI) observations and Weather Research and Forecasting (WRF)-Community Multiscale Air Quality (CMAQ) model simulations. An algorithm was developed based on mass conservation to estimate the 30 km × 30 km resolved top-down NOx emissions over East Asia. In particular, the algorithm developed in this study considered two main atmospheric factors—(i) NOx transport from/to adjacent cells and (ii) calculations of the lifetimes of column NOx (τ). In the sensitivity test, the analysis showed the improvements in the top-down NOx estimation via filtering the data (τ ≤ 2 h). The best top-down NOx emissions were inferred after the sixth iterations. Those emissions were 11.76 Tg N yr−1 over China, 0.13 Tg N yr−1 over North Korea, 0.46 Tg N yr−1 over South Korea, and 0.68 Tg N yr−1 over Japan. These values are 34%, 62%, 60%, and 47% larger than the current bottom-up NOx emissions over these countries, respectively. A comparison between the CMAQ-estimated and OMI-retrieved NO2 columns was made to confirm the accuracy of the newly estimated NOx emission. The comparison confirmed that the estimated top-down NOx emissions showed better agreements with observations (R2 = 0.88 for January and 0.81 for July).

scholarly journals Worldwide biogenic soil NO<sub>x</sub> emissions inferred from OMI NO<sub>2</sub> observations

2014 ◽  
Vol 14 (18) ◽  
pp. 10363-10381 ◽  
Author(s):  
G. C. M. Vinken ◽  
K. F. Boersma ◽  
J. D. Maasakkers ◽  
M. Adon ◽  
R. V. Martin
Keyword(s):  
Emission Inventory ◽  
Transport Model ◽  
A Priori ◽  
Nox Emission ◽  
Nox Emissions ◽  
Ozone Monitoring Instrument ◽  
Top Down ◽  
Tropospheric No2 ◽  
The Usa ◽  
Time Specific

Abstract. Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 15 Tg N yr−1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). We use a state-of-science soil NOx emission inventory (Hudman et al., 2012) as a priori in the GEOS-Chem chemistry transport model to identify 11 regions where tropospheric NO2 columns are dominated by soil NOx emissions. Strong correlations between soil NOx emissions and simulated NO2 columns indicate that spatial patterns in simulated NO2 columns in these regions indeed reflect the underlying soil NOx emissions. Subsequently, we use a mass-balance approach to constrain emissions for these 11 regions on all major continents using OMI observed and GEOS-Chem simulated tropospheric NO2 columns. We find that responses of simulated NO2 columns to changing NOx emissions are suppressed over low NOx regions, and account for these non-linearities in our inversion approach. In general, our approach suggests that emissions need to be increased in most regions. Our OMI top-down soil NOx inventory amounts to 10.0 Tg N for 2005 when only constraining the 11 regions, and 12.9 Tg N when extrapolating the constraints globally. Substantial regional differences exist (ranging from −40% to +90%), and globally our top-down inventory is 4–35% higher than the GEOS-Chem a priori (9.6 Tg N yr−1). We evaluate NO2 concentrations simulated with our new OMI top-down inventory against surface NO2 measurements from monitoring stations in Africa, the USA and Europe. Although this comparison is complicated by several factors, we find an encouraging improved agreement when using the OMI top-down inventory compared to using the a priori inventory. To our knowledge, this study provides, for the first time, specific constraints on soil NOx emissions on all major continents using OMI NO2 columns. Our results rule out the low end of reported soil NOx emission estimates, and suggest that global emissions are most likely around 12.9 ± 3.9 Tg N yr−1.

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