scholarly journals Unraveling Pathways of Elevated Ozone Induced by the 2020 Lockdown in Europe by an Observationally Constrained Regional Model: Non-Linear Joint Inversion of NO<sub>x</sub> and VOC Emissions using TROPOMI

2021 ◽  
Author(s):  
Amir H. Souri ◽  
Kelly Chance ◽  
Juseon Bak ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
...  
Keyword(s):  
Central Europe ◽  
Joint Inversion ◽  
Surface Ozone ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Nox Emissions ◽  
Physical Processes ◽  
Model Estimate ◽  
Large Variability ◽  
Voc Emissions

Abstract. Questions about how emissions are changing during the COVID-19 lockdown periods cannot be answered by observations of atmospheric trace gas concentrations alone, in part due to simultaneous changes in atmospheric transport, emissions, dynamics, photochemistry, and chemical feedback. A chemical transport model simulation benefiting from a multi-species inversion framework using well-characterized observations should differentiate those influences enabling to closely examine changes in emissions. This approach has another advantage in that we can, to a certain extent, disentangle the chemical and physical processes involved in the formation of ozone. Accordingly, we jointly constrain NOx and VOC emissions using well-characterized TROPOMI HCHO and NO2 columns during the months of March, April, and May 2020 (lockdown) and 2019 (baseline). We observe a noticeable decline in the magnitude of NOx emissions in March 2020 (14–31 %) in several major cities including Paris, London, Madrid, and Milan expanding further to Rome, Brussels, Frankfurt, Warsaw, Belgrade, Kyiv, and Moscow (34–51 %) in April. The large variability of changes in NOx emissions is indicative of different dates and the degree of restrictions enacted to prevent the spread of the virus. For instance, NOx emissions remain at somewhat similar values or even higher in northern Germany and Moscow in March 2020 compared to the baseline. Comparisons against surface monitoring stations indicate that the model estimate of the NO2 reduction is underestimated, a picture that correlates with the TROPOMI frequency impacted by cloudiness. During the month of April, when ample TROPOMI samples are present, the surface NO2 reductions occurring in polluted areas are described fairly well by the model (model: −21 ± 17 %, observation: −29 ± 21 %). Changes in VOC emissions are dominated by eastern European biomass burning activities and biogenic isoprene emissions. In March, however, TROPOMI HCHO sets an upper limit for HCHO changes such that the chemical feedback of NOx on HCHO constrained by TROPOMI NO2 reveals a non-negligible decline in anthropogenic VOC emissions in Paris (−9 %), Milan (−29 %), London (−5 %), and Rome (−5 %). Results support an increase in surface ozone during the lockdown. In April, the constrained model features a reasonable agreement with maximum daily 8 h average (MDA8) ozone changes observed at the surface (r = 0.43), specifically over central Europe where ozone enhancements prevail (model: +3.73 ± 3.94 %, +1.79 ppbv, observation: +7.35 ± 11.27 %, +3.76 ppbv). Results of integrated process rates of MDA8 surface ozone over central Europe in the same month suggest that physical processes (dry deposition, advection and diffusion) decrease ozone on average by −4.83 ppbv, while ozone production rates dampened by largely negative JNO2[NO2]-kNO+O3[NO][O3] become less negative, leading ozone to increase by +5.89 ppbv. Experiments involving fixed anthropogenic emissions suggest that meteorology (mainly as air temperature and photolysis) contributes to 42 % enhancement in MDA8 surface ozone over the same region with the remaining part (58 %) coming from changes in anthropogenic emissions. Results illustrate the capability of satellite data of major ozone precursors to help atmospheric models capture the essential character of ozone changes induced by abrupt emission anomalies.

scholarly journals Unraveling pathways of elevated ozone induced by the 2020 lockdown in Europe by an observationally constrained regional model using TROPOMI

2021 ◽  
Vol 21 (24) ◽  
pp. 18227-18245
Author(s):  
Amir H. Souri ◽  
Kelly Chance ◽  
Juseon Bak ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
...  
Keyword(s):  
Transport Model ◽  
Atmospheric Transport ◽  
Model Simulation ◽  
Surface Ozone ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Nox Emissions ◽  
Chemical Transport Model ◽  
Voc Emissions ◽  
Constrained Model

Abstract. Questions about how emissions are changing during the COVID-19 lockdown periods cannot be answered by observations of atmospheric trace gas concentrations alone, in part due to simultaneous changes in atmospheric transport, emissions, dynamics, photochemistry, and chemical feedback. A chemical transport model simulation benefiting from a multi-species inversion framework using well-characterized observations should differentiate those influences enabling to closely examine changes in emissions. Accordingly, we jointly constrain NOx and VOC emissions using well-characterized TROPOspheric Monitoring Instrument (TROPOMI) HCHO and NO2 columns during the months of March, April, and May 2020 (lockdown) and 2019 (baseline). We observe a noticeable decline in the magnitude of NOx emissions in March 2020 (14 %–31 %) in several major cities including Paris, London, Madrid, and Milan, expanding further to Rome, Brussels, Frankfurt, Warsaw, Belgrade, Kyiv, and Moscow (34 %–51 %) in April. However, NOx emissions remain at somewhat similar values or even higher in some portions of the UK, Poland, and Moscow in March 2020 compared to the baseline, possibly due to the timeline of restrictions. Comparisons against surface monitoring stations indicate that the constrained model underrepresents the reduction in surface NO2. This underrepresentation correlates with the TROPOMI frequency impacted by cloudiness. During the month of April, when ample TROPOMI samples are present, the surface NO2 reductions occurring in polluted areas are described fairly well by the model (model: −21 ± 17 %, observation: −29 ± 21 %). The observational constraint on VOC emissions is found to be generally weak except for lower latitudes. Results support an increase in surface ozone during the lockdown. In April, the constrained model features a reasonable agreement with maximum daily 8 h average (MDA8) ozone changes observed at the surface (r=0.43), specifically over central Europe where ozone enhancements prevail (model: +3.73 ± 3.94 %, +1.79 ppbv, observation: +7.35 ± 11.27 %, +3.76 ppbv). The model suggests that physical processes (dry deposition, advection, and diffusion) decrease MDA8 surface ozone in the same month on average by −4.83 ppbv, while ozone production rates dampened by largely negative JNO2[NO2]-kNO+O3[NO][O3] become less negative, leading ozone to increase by +5.89 ppbv. Experiments involving fixed anthropogenic emissions suggest that meteorology contributes to 42 % enhancement in MDA8 surface ozone over the same region with the remaining part (58 %) coming from changes in anthropogenic emissions. Results illustrate the capability of satellite data of major ozone precursors to help atmospheric models capture ozone changes induced by abrupt emission anomalies.

scholarly journals The influence of temperature on ozone production under varying NO<sub><i>x</i></sub> conditions – a modelling study

2016 ◽  
Vol 16 (18) ◽  
pp. 11601-11615 ◽  
Author(s):  
Jane Coates ◽  
Kathleen A. Mar ◽  
Narendra Ojha ◽  
Tim M. Butler
Keyword(s):  
Central Europe ◽  
Surface Ozone ◽  
Reaction Rates ◽  
Air Pollutant ◽  
Box Model ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
Nox Emissions ◽  
Model Simulations ◽  
Rate Of Increase

Abstract. Surface ozone is a secondary air pollutant produced during the atmospheric photochemical degradation of emitted volatile organic compounds (VOCs) in the presence of sunlight and nitrogen oxides (NOx). Temperature directly influences ozone production through speeding up the rates of chemical reactions and increasing the emissions of VOCs, such as isoprene, from vegetation. In this study, we used an idealised box model with different chemical mechanisms (Master Chemical Mechanism, MCMv3.2; Common Representative Intermediates, CRIv2; Model for OZone and Related Chemical Tracers, MOZART-4; Regional Acid Deposition Model, RADM2; Carbon Bond Mechanism, CB05) to examine the non-linear relationship between ozone, NOx and temperature, and we compared this to previous observational studies. Under high-NOx conditions, an increase in ozone from 20 to 40 °C of up to 20 ppbv was due to faster reaction rates, while increased isoprene emissions added up to a further 11 ppbv of ozone. The largest inter-mechanism differences were obtained at high temperatures and high-NOx emissions. CB05 and RADM2 simulated more NOx-sensitive chemistry than MCMv3.2, CRIv2 and MOZART-4, which could lead to different mitigation strategies being proposed depending on the chemical mechanism. The increased oxidation rate of emitted VOC with temperature controlled the rate of Ox production; the net influence of peroxy nitrates increased net Ox production per molecule of emitted VOC oxidised. The rate of increase in ozone mixing ratios with temperature from our box model simulations was about half the rate of increase in ozone with temperature observed over central Europe or simulated by a regional chemistry transport model. Modifying the box model set-up to approximate stagnant meteorological conditions increased the rate of increase of ozone with temperature as the accumulation of oxidants enhanced ozone production through the increased production of peroxy radicals from the secondary degradation of emitted VOCs. The box model simulations approximating stagnant conditions and the maximal ozone production chemical regime reproduced the 2 ppbv increase in ozone per degree Celsius from the observational and regional model data over central Europe. The simulated ozone–temperature relationship was more sensitive to mixing than the choice of chemical mechanism. Our analysis suggests that reductions in NOx emissions would be required to offset the additional ozone production due to an increase in temperature in the future.

scholarly journals Low modeled ozone production suggests underestimation of precursor emissions (especially NO<sub><i>x</i></sub>) in Europe

2018 ◽  
Vol 18 (3) ◽  
pp. 2175-2198 ◽  
Author(s):  
Emmanouil Oikonomakis ◽  
Sebnem Aksoyoglu ◽  
Giancarlo Ciarelli ◽  
Urs Baltensperger ◽  
André Stephan Henry Prévôt
Keyword(s):  
Air Quality ◽  
Surface Ozone ◽  
Model Performance ◽  
Ozone Production ◽  
Nox Emissions ◽  
Air Quality Model ◽  
Quality Model ◽  
Voc Emissions ◽  
Mixing Ratios ◽  
The Impact

Abstract. High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modeling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone–temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, the Comprehensive Air Quality Model with Extensions (CAMx). The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (≥ 60 ppb) by 10–20 ppb and overestimates the lower ones (< 40 ppb) by 5–15 ppb, resulting in a misleading good agreement with the observations for average ozone. The model also underestimates the ozone–temperature regression slope by about a factor of 2 for most of the measurement stations. To investigate the impact of emissions, four scenarios were tested: (i) increased volatile organic compound (VOC) emissions by a factor of 1.5 and 2 for the anthropogenic and biogenic VOC emissions, respectively, (ii) increased nitrogen oxide (NOx) emissions by a factor of 2, (iii) a combination of the first two scenarios and (iv) increased traffic-only NOx emissions by a factor of 4. For southern, eastern, and central (except the Benelux area) Europe, doubling NOx emissions seems to be the most efficient scenario to reduce the underestimation of the observed high ozone mixing ratios without significant degradation of the model performance for the lower ozone mixing ratios. The model performance for ozone–temperature correlation is also better when NOx emissions are doubled. In the Benelux area, however, the third scenario (where both NOx and VOC emissions are increased) leads to a better model performance. Although increasing only the traffic NOx emissions by a factor of 4 gave very similar results to the doubling of all NOx emissions, the first scenario is more consistent with the uncertainties reported by other studies than the latter, suggesting that high uncertainties in NOx emissions might originate mainly from the road-transport sector rather than from other sectors. The impact of meteorology was examined with three sensitivity tests: (i) increased surface temperature by 4 ∘C, (ii) reduced wind speed by 50 % and (iii) doubled wind speed. The first two scenarios led to a consistent increase in all surface ozone mixing ratios, thus improving the model performance for the high ozone values but significantly degrading it for the low ozone values, while the third scenario had exactly the opposite effects. Overall, the modeled ozone is predicted to be more sensitive to its precursor emissions (especially traffic NOx) and therefore their uncertainties, which seem to be responsible for the model underestimation of the observed high ozone mixing ratios and ozone production.

scholarly journals An Inversion of NO<sub><i>x</i></sub> and NMVOC Emissions using Satellite Observations during the KORUS-AQ Campaign and Implications for Surface Ozone over East Asia

2020 ◽  
Author(s):  
Amir H. Souri ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
Lei Zhu ◽  
Donald R. Blake ◽  
...  
Keyword(s):  
East Asia ◽  
Power Plants ◽  
Surface Ozone ◽  
Thermal Power ◽  
River Delta ◽  
Ozone Production ◽  
Nox Emissions ◽  
Voc Emissions ◽  
Non Linear ◽  
The Impact

Abstract. The absence of up-to-date emissions has been a major impediment to accurately simulate aspects of atmospheric chemistry, and to precisely quantify the impact of changes of emissions on air pollution. Hence, a non-linear joint analytical inversion (Gauss–Newton method) of both volatile organic compounds (VOC) and nitrogen oxides (NOx) emissions is made by exploiting the Smithsonian Astrophysical Observatory (SAO) Ozone Mapping and Profile Suite Nadir Mapper (OMPS-NM) formaldehyde (HCHO) and the National Aeronautics and Space Administration (NASA) Ozone Monitoring Instrument (OMI) tropospheric nitrogen dioxide (NO2) retrievals during the Korea-United States Air Quality (KORUS-AQ) campaign over East Asia in May–June 2016. Effects of the chemical feedback of NOx and VOCs on both NO2 and HCHO are implicitly included through iteratively optimizing the inversion. Emissions estimates are greatly improved (averaging kernels > 0.8) over medium- to high-emitting areas such as cities and dense vegetation. The amount of total NOx emissions is mainly dictated by values reported in the MIX-Asia 2010 inventory. After the inversion we conclude a decline in the emissions (before, after, change) for China (87.94 ± 44.09 Gg/day, 68.00 ± 15.94 Gg/day, −23 %), North China Plain (NCP) (27.96 ± 13.49 Gg/day, 19.05 ± 2.50 Gg/day, −32 %), Pearl River Delta (PRD) (4.23 ± 1.78 Gg/day, 2.70 ± 0.32 Gg/day, −36 %), Yangtze River Delta (YRD) (9.84 ± 4.68 Gg/day, 5.77 ± 0.51 Gg/day, −41 %), Taiwan (1.26 ± 0.57 Gg/day, 0.97 ± 0.33 Gg/day, −23 %), and Malaysia (2.89 ± 2.77 Gg/day, 2.25 ± 1.34 Gg/day, −22 %), all of which have effectively implemented various stringent regulations. In contrast, South Korea (2.71 ± 1.34 Gg/day, 2.95 ± 0.58 Gg/day, +9 %) and Japan (3.53 ± 1.71 Gg/day, 3.96 ± 1.04 Gg/day, +12 %) experience an increase in NOx emissions potentially due to risen number of diesel vehicles and new thermal power plants. We revisit the well-documented positive bias of the model in terms of biogenic VOC emissions in the tropics. The inversion, however, suggests a larger growth of VOC (mainly anthropogenic) over NCP (25 %) than previously reported (6 %) relative to 2010. The spatial variation in both magnitude and sign of NOx and VOC emissions results in non-linear responses of ozone production/loss. Due to simultaneous decrease/increase of NOx/VOC over NCP and YRD, we observe an ~ 53 % reduction in the ratio of the chemical loss of NOx (LNOx) to the chemical loss of ROx (RO2 + HO2) transitioning toward NOx-sensitive regimes, which in turn, reduces/increases the afternoon chemical loss/production of ozone through NO2 + OH (−0.42 ppbv hr−1)/HO2 (and RO2) + NO (+0.31 ppbv hr−1). Conversely, a combined decrease in NOx and VOC emissions in Taiwan, Malaysia, and the southern China suppresses the formation of ozone. Ultimately, model simulations indicate enhancements of maximum daily 8-hour average (MDA8) surface ozone over China (0.62 ppbv), NCP (4.56 ppbv), and YRD (5.25 ppbv) due to the non-linear ozone chemistry, suggesting that emissions standards should be extended to regulate VOCs to be able to curb ozone production rates. Taiwan, Malaysia, and PRD stand out as the regions undergoing lower MDA8 ozone levels resulting from the NOx reductions occurring predominantly in NOx-sensitive regimes.

scholarly journals An inversion of NO<sub><i>x</i></sub> and non-methane volatile organic compound (NMVOC) emissions using satellite observations during the KORUS-AQ campaign and implications for surface ozone over East Asia

2020 ◽  
Vol 20 (16) ◽  
pp. 9837-9854 ◽  
Author(s):  
Amir H. Souri ◽  
Caroline R. Nowlan ◽  
Gonzalo González Abad ◽  
Lei Zhu ◽  
Donald R. Blake ◽  
...  
Keyword(s):  
East Asia ◽  
Surface Ozone ◽  
Thermal Power ◽  
Satellite Observations ◽  
River Delta ◽  
Ozone Production ◽  
Nox Emissions ◽  
Voc Emissions ◽  
Volatile Organic ◽  
The Impact

Abstract. The absence of up-to-date emissions has been a major impediment to accurately simulating aspects of atmospheric chemistry and to precisely quantifying the impact of changes in emissions on air pollution. Hence, a nonlinear joint analytical inversion (Gauss–Newton method) of both volatile organic compounds (VOCs) and nitrogen oxide (NOx) emissions is made by exploiting the Smithsonian Astrophysical Observatory (SAO) Ozone Mapping and Profiler Suite Nadir Mapper (OMPS-NM) formaldehyde (HCHO) and the National Aeronautics and Space Administration (NASA) Ozone Monitoring Instrument (OMI) tropospheric nitrogen dioxide (NO2) columns during the Korea–United States Air Quality (KORUS-AQ) campaign over East Asia in May–June 2016. Effects of the chemical feedback of NOx and VOCs on both NO2 and HCHO are implicitly included by iteratively optimizing the inversion. Emission uncertainties are greatly narrowed (averaging kernels > 0.8, which is the mathematical presentation of the partition of information gained from the satellite observations with respect to the prior knowledge) over medium- to high-emitting areas such as cities and dense vegetation. The prior amount of total NOx emissions is mainly dictated by values reported in the MIX-Asia 2010 inventory. After the inversion we conclude that there is a decline in emissions (before, after, change) for China (87.94±44.09 Gg d−1, 68.00±15.94 Gg d−1, −23 %), North China Plain (NCP) (27.96±13.49 Gg d−1, 19.05±2.50 Gg d−1, −32 %), Pearl River Delta (PRD) (4.23±1.78 Gg d−1, 2.70±0.32 Gg d−1, −36 %), Yangtze River Delta (YRD) (9.84±4.68 Gg d−1, 5.77±0.51 Gg d−1, −41 %), Taiwan (1.26±0.57 Gg d−1, 0.97±0.33 Gg d−1, −23 %), and Malaysia (2.89±2.77 Gg d−1, 2.25±1.34 Gg d−1, −22 %), all of which have effectively implemented various stringent regulations. In contrast, South Korea (2.71±1.34 Gg d−1, 2.95±0.58 Gg d−1, +9 %) and Japan (3.53±1.71 Gg d−1, 3.96±1.04 Gg d−1, +12 %) are experiencing an increase in NOx emissions, potentially due to an increased number of diesel vehicles and new thermal power plants. We revisit the well-documented positive bias (by a factor of 2 to 3) of MEGAN v2.1 (Model of Emissions of Gases and Aerosols from Nature) in terms of biogenic VOC emissions in the tropics. The inversion, however, suggests a larger growth of VOCs (mainly anthropogenic) over NCP (25 %) than previously reported (6 %) relative to 2010. The spatial variation in both the magnitude and sign of NOx and VOC emissions results in nonlinear responses of ozone production and loss. Due to a simultaneous decrease and increase in NOx∕VOC over NCP and YRD, we observe a ∼53 % reduction in the ratio of the chemical loss of NOx (LNOx) to the chemical loss of ROx (RO2+HO2) over the surface transitioning toward NOx-sensitive regimes, which in turn reduces and increases the afternoon chemical loss and production of ozone through NO2+OH (−0.42 ppbv h−1)∕HO2 (and RO2)+NO (+0.31 ppbv h−1). Conversely, a combined decrease in NOx and VOC emissions in Taiwan, Malaysia, and southern China suppresses the formation of ozone. Simulations using the updated emissions indicate increases in maximum daily 8 h average (MDA8) surface ozone over China (0.62 ppbv), NCP (4.56 ppbv), and YRD (5.25 ppbv), suggesting that emission control strategies on VOCs should be prioritized to curb ozone production rates in these regions. Taiwan, Malaysia, and PRD stand out as regions undergoing lower MDA8 ozone levels resulting from the NOx reductions occurring predominantly in NOx-sensitive regimes.

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 TOAST 1.0: Tropospheric Ozone Attribution of Sources with Tagging for CESM 1.2.2

2018 ◽  
Vol 11 (7) ◽  
pp. 2825-2840 ◽  
Author(s):  
Tim Butler ◽  
Aurelia Lupascu ◽  
Jane Coates ◽  
Shuai Zhu
Keyword(s):  
Tropospheric Ozone ◽  
Surface Ozone ◽  
Chemical Mechanism ◽  
System Model ◽  
Ozone Production ◽  
Anthropogenic Emissions ◽  
Source Attribution ◽  
Volatile Organic ◽  
Community Earth System Model ◽  
Northern Hemispheric

Abstract. A system for source attribution of tropospheric ozone produced from both NOx and volatile organic compound (VOC) precursors is described, along with its implementation in the Community Earth System Model (CESM) version 1.2.2 using CAM4. The user can specify an arbitrary number of tag identities for each NOx or VOC species in the model, and the tagging system rewrites the model chemical mechanism and source code to incorporate tagged tracers and reactions representing these tagged species, as well as ozone produced in the stratosphere. If the user supplies emission files for the corresponding tagged tracers, the model will produce tagged ozone tracers which represent the contribution of each of the tag identities to the modelled total tropospheric ozone. Our tagged tracers preserve Ox. The size of the tagged chemical mechanism scales linearly with the number of specified tag identities. Separate simulations are required for NOx and VOC tagging, which avoids the sharing of tag identities between NOx and VOC species. Results are presented and evaluated for both NOx and VOC source attribution. We show that northern hemispheric surface ozone is dominated year-round by anthropogenic emissions of NOx, but that the mix of corresponding VOC precursors changes over the course of the year; anthropogenic VOC emissions contribute significantly to surface ozone in winter–spring, while biogenic VOCs are more important in summer. The system described here can provide important diagnostic information about modelled ozone production, and could be used to construct source–receptor relationships for tropospheric ozone.

scholarly journals Sensitivities of NO<sub>x</sub> transformation and the effects on surface ozone and nitrate

2014 ◽  
Vol 14 (3) ◽  
pp. 1385-1396 ◽  
Author(s):  
H. Lei ◽  
J. X. L. Wang
Keyword(s):  
Air Quality ◽  
Los Angeles ◽  
Surface Ozone ◽  
Nox Emission ◽  
Ozone Production ◽  
Limited Area ◽  
Transformation Rate ◽  
Nox Emissions ◽  
Increase Rate ◽  
Industrial Regions

Abstract. As precursors to tropospheric ozone and nitrate, nitrogen oxide (NOx) in the present atmosphere and its transformation in response to emission and climate perturbations are studied by using the CAM-Chem model and air quality measurements from the National Emissions Inventory (NEI), Clean Air Status and Trends Network (CASTNET), and Environmental Protection Agency Air Quality System (EPA AQS). It is found that NOx transformations in present atmospheric conditions show different sensitivities over industrial and non-industrial regions. As a result, the surface ozone and nitrate formations can be divided into several regimes associated with the dominant emission types and relative levels of NOx and volatile organic compounds (VOC). Ozone production in industrial regions (the main NOx emission source areas) increases in warmer conditions and slightly decreases following an increase in NOx emissions due to NOx titration, which is opposite to the response in non-industrial regions. The ozone decrease following a temperature increase in non-industrial regions indicates that ozone production in regions that lack NOx emission sources may be sensitive to NOx transformation in remote source regions. The increase in NO2 from NOx titration over industrial regions results in an increase rate of total nitrate that remains higher than the increase rate of NOx emissions. The presented findings indicate that a change in the ozone concentration is more directly affected by changes in climate and precursor emissions, while a change in the nitrate concentration is affected by local ozone production types and their seasonal transfer. The sensitivity to temperature perturbations shows that a warmer climate accelerates the decomposition of odd nitrogen (NOy) during the night. As a result, the transformation rate of NOx to nitrate decreases. Examinations of the historical emissions and air quality records of a typical NOx-limited area, such as Atlanta and a VOC-limited area, such as Los Angeles further confirm the conclusions drawn from the modeling experiments.

scholarly journals Tropospheric ozone changes and ozone sensitivity from present-day to future under shared socio-economic pathways

2021 ◽  
Author(s):  
Zhenze Liu ◽  
Ruth M. Doherty ◽  
Oliver Wild ◽  
Fiona M. O’Connor ◽  
Steven T. Turnock
Keyword(s):  
North America ◽  
Tropospheric Ozone ◽  
Surface Ozone ◽  
Nox Emissions ◽  
Limited Region ◽  
Voc Emissions ◽  
Ozone Concentrations ◽  
Ozone Sensitivity ◽  
The Future ◽  
High Emission

Abstract. Tropospheric ozone is important to future air quality and climate. We investigate ozone changes and ozone sensitivity to changing emissions in the context of climate change from the present day (2004–2014) to the future (2045–2055) under a range of shared socio-economic pathways (SSPs). We apply the United Kingdom Earth System Model, UKESM1, with an extended chemistry scheme including more reactive volatile organic compounds (VOCs) to quantify ozone burdens as well as ozone sensitivities globally and regionally based on nitrogen oxide (NOx) and VOC concentrations. We show that the tropospheric ozone burden increases by 4 % under a development pathway with higher NOx and VOC emissions (SSP3-7.0), but decreases by 7 % under the same pathway if NOx and VOC emissions are reduced (SSP3-7.0-lowNTCF) and by 5 % if atmospheric methane (CH4) concentrations are reduced (SSP3-7.0-lowCH4). Global mean surface ozone concentrations are reduced by 3–5 ppb under SSP3-7.0-lowNTCF and by 2–3 ppb under SSP3-7.0-lowCH4. However, surface ozone changes vary substantially by season in high-emission regions under future pathways, with decreased ozone concentrations in summer and increased ozone concentrations in winter when NOx emissions are reduced. VOC-limited areas are more extensive in winter (7 %) than in summer (3 %) across the globe. North America, Europe and East Asia are the dominant VOC-limited regions in the present day but North America and Europe become more NOx-limited in the future mainly due to reductions in NOx emissions. The impacts of VOC emissions on O3 sensitivity are limited in North America and Europe because reduced anthropogenic VOC emissions are offset by higher biogenic VOC emissions. O3 sensitivity is not greatly influenced by changing CH4 concentrations. South Asia becomes the dominant VOC-limited region under future pathways. We highlight that reductions in NOx emissions are required to transform O3 production from VOC- to NOx-limitation, but that these lead to increased O3 concentrations in high-emission regions, and hence emission controls on VOC and CH4 are also necessary.

scholarly journals Effect of regional precursor emission controls on long-range ozone transport – Part 1: short-term changes in ozone air quality

2009 ◽  
Vol 9 (2) ◽  
pp. 7033-7077
Author(s):  
J. J. West ◽  
V. Naik ◽  
L. W. Horowitz ◽  
A. M. Fiore
Keyword(s):  
Air Quality ◽  
Long Range ◽  
Surface Ozone ◽  
Source Region ◽  
Lower Troposphere ◽  
Ozone Production ◽  
Nox Emissions ◽  
Short Term ◽  
Source Regions ◽  
Ozone Transport

Abstract. Observations and models demonstrate that ozone and its precursors can be transported between continents and across oceans. We model the influences of 10% reductions in anthropogenic nitrogen oxide (NOx) emissions from each of nine world regions on surface ozone air quality in that region and all other regions. In doing so, we quantify the relative importance of long-range transport between all source-receptor pairs, for direct short-term ozone changes. We find that for population-weighted concentrations during the three-month "ozone-season", the strongest inter-regional influences are from Europe to the Former Soviet Union, East Asia to Southeast Asia, and Europe to Africa. The largest influences per unit of NOx reduced, however, are seen for source regions in the tropics and Southern Hemisphere, which we attribute mainly to greater sensitivity to changes in NOx in the lower troposphere, and secondarily to increased vertical convection to the free troposphere in tropical regions, allowing pollutants to be transported further. Results show, for example, that NOx reductions in North America are ~20% as effective per unit NOx in reducing ozone in Europe during summer, as NOx reductions from Europe itself. Reducing anthropogenic emissions of non-methane volatile organic compounds (NMVOCs) and carbon monoxide (CO) by 10% in selected regions, can have as large an impact on long-range ozone transport as NOx reductions, depending on the source region. We find that for many source-receptor pairs, the season of greatest long-range influence does not coincide with the season when ozone is highest in the receptor region. Reducing NOx emissions in most source regions causes a larger decrease in export of ozone from the source region than in ozone production outside of the source region.

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