scholarly journals Ozone impacts of gas–aerosol uptake in global chemistry transport models

2018 ◽  
Vol 18 (5) ◽  
pp. 3147-3171 ◽  
Author(s):  
Scarlet Stadtler ◽  
David Simpson ◽  
Sabine Schröder ◽  
Domenico Taraborrelli ◽  
Andreas Bott ◽  
...  
Keyword(s):  
East Asia ◽  
Surface Area ◽  
General Circulation ◽  
Heterogeneous Reaction ◽  
Circulation Model ◽  
Photochemical Reactions ◽  
Heterogeneous Reactions ◽  
Transport Models ◽  
Global Pattern ◽  
The Impact

Abstract. The impact of six heterogeneous gas–aerosol uptake reactions on tropospheric ozone and nitrogen species was studied using two chemical transport models, the Meteorological Synthesizing Centre-West of the European Monitoring and Evaluation Programme (EMEP MSC-W) and the European Centre Hamburg general circulation model combined with versions of the Hamburg Aerosol Model and Model for Ozone and Related chemical Tracers (ECHAM-HAMMOZ). Species undergoing heterogeneous reactions in both models include N2O5, NO3, NO2, O3, HNO3, and HO2. Since heterogeneous reactions take place at the aerosol surface area, the modelled surface area density (Sa) of both models was compared to a satellite product retrieving the surface area. This comparison shows a good agreement in global pattern and especially the capability of both models to capture the extreme aerosol loadings in east Asia. The impact of the heterogeneous reactions was evaluated by the simulation of a reference run containing all heterogeneous reactions and several sensitivity runs. One reaction was turned off in each sensitivity run to compare it with the reference run. The analysis of the sensitivity runs confirms that the globally most important heterogeneous reaction is the one of N2O5. Nevertheless, NO2, HNO3, and HO2 heterogeneous reactions gain relevance particularly in east Asia due to the presence of high NOx concentrations and high Sa in the same region. The heterogeneous reaction of O3 itself on dust is of minor relevance compared to the other heterogeneous reactions. The impacts of the N2O5 reactions show strong seasonal variations, with the biggest impacts on O3 in springtime when photochemical reactions are active and N2O5 levels still high. Evaluation of the models with northern hemispheric ozone surface observations yields a better agreement of the models with observations in terms of concentration levels, variability, and temporal correlations at most sites when the heterogeneous reactions are incorporated. Our results are loosely consistent with results from earlier studies, although the magnitude of changes induced by N2O5 reaction is at the low end of estimates, which seems to fit a trend, whereby the more recent the study the lower the impacts of these reactions.

scholarly journals Ozone Impacts of Gas-Aerosol Uptake in Global Chemistry Transport Models

2017 ◽  
Author(s):  
Scarlet Stadtler ◽  
David Simpson ◽  
Sabine Schröder ◽  
Domenico Taraborrelli ◽  
Andreas Bott ◽  
...  
Keyword(s):  
East Asia ◽  
Surface Area ◽  
Heterogeneous Reaction ◽  
Photochemical Reactions ◽  
Heterogeneous Reactions ◽  
Transport Models ◽  
Global Pattern ◽  
Temporal Correlations ◽  
The One ◽  
The Impact

Abstract. The impact of six heterogeneous gas-aerosol uptake reactions on tropospheric ozone and nitrogen species was studied using two chemical transport models, EMEP MSC-W and ECHAM-HAMMOZ. Species undergoing heterogeneous reactions in both models include N2O5, NO3, NO2, O3, HNO3 and HO2. Since heterogeneous reactions take place at the aerosol surface area, the modeled surface area density Sa of both models was compared to a satellite product retrieving the surface area. This comparison shows a good agreement in global pattern and especially the capability of both models to capture the extreme aerosol loadings in East Asia. The impact of the heterogeneous reactions was evaluated by the simulation of a reference run containing all heterogeneous reactions and several sensitivity runs. One reaction was turned off in each sensitivity run to compare it with the reference run. The analysis of the sensitivity runs confirms that the globally most important heterogeneous reaction is the one of N2O5. Nevertheless, NO2, HNO3 and HO2 heterogeneous reaction gain relevance particularly in East Asia due to the presence of high NOx concentrations and high Sa in the same region, although ECHAM-HAMMOZ showed much stronger responses than EMEP in this respect. The heterogeneous reaction of O3 itself on dust is of minor relevance compared to the other heterogeneous reactions. The impacts of the N2O5 reactions show strong seasonal variations, with biggest impacts on O3 in spring time when photochemical reactions are active and N2O5 levels still high. Evaluation of the models with northern hemispheric ozone surface observations yields a better agreement of the models with observations in terms of concentration levels, variability, and temporal correlations at most sites when the heterogeneous reactions are incorporated.

scholarly journals Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing, China

2019 ◽  
Vol 19 (10) ◽  
pp. 6737-6747 ◽  
Author(s):  
Xionghui Qiu ◽  
Qi Ying ◽  
Shuxiao Wang ◽  
Lei Duan ◽  
Jian Zhao ◽  
...  
Keyword(s):  
Heterogeneous Reaction ◽  
Particle Surface ◽  
Heterogeneous Reactions ◽  
Sensitivity Analyses ◽  
Uptake Coefficient ◽  
Transport Models ◽  
Nitrate Concentrations ◽  
The Impact ◽  
Beijing China ◽  
Significant Underestimation

Abstract. Comprehensive chlorine heterogeneous chemistry is incorporated into the Community Multiscale Air Quality (CMAQ) model to evaluate the impact of chlorine-related heterogeneous reaction on diurnal and nocturnal nitrate formation and quantify the nitrate formation from gas-to-particle partitioning of HNO3 and from different heterogeneous pathways. The results show that these heterogeneous reactions increase the atmospheric Cl2 and ClNO2 level (∼ 100 %), which further affects the nitrate formation. Sensitivity analyses of uptake coefficients show that the empirical uptake coefficient for the O3 heterogeneous reaction with chlorinated particles may lead to the large uncertainties in the predicted Cl2 and nitrate concentrations. The N2O5 uptake coefficient with particulate Cl− concentration dependence performs better in capturing the concentration of ClNO2 and nocturnal nitrate concentration. The reaction of OH and NO2 in the daytime increases the nitrate by ∼15 % when the heterogeneous chlorine chemistry is incorporated, resulting in more nitrate formation from HNO3 gas-to-particle partitioning. By contrast, the contribution of the heterogeneous reaction of N2O5 to nitrate concentrations decreases by about 27 % in the nighttime, when its reactions with chlorinated particles are considered. However, the generated gas-phase ClNO2 from the heterogeneous reaction of N2O5 and chlorine-containing particles further reacts with the particle surface to increase the nitrate by 6 %. In general, this study highlights the potential of significant underestimation of daytime concentrations and overestimation of nighttime nitrate concentrations for chemical transport models without proper chlorine chemistry in the gas and particle phases.

scholarly journals Terrestrial sources and distribution of atmospheric sulphur

1997 ◽  
Vol 352 (1350) ◽  
pp. 149-158 ◽  
Author(s):  
J. Lelieveld ◽  
G.–J. Roelofs ◽  
L. Ganzeveld ◽  
J. Feichter ◽  
H. Rodhe
Keyword(s):  
Aqueous Phase ◽  
General Circulation ◽  
Heterogeneous Reaction ◽  
Circulation Model ◽  
Anthropogenic Emissions ◽  
Natural Emissions ◽  
Global Estimates ◽  
Deposition Processes ◽  
The Impact ◽  
Sulphur Species

The general circulation model ECHAM has been coupled to a chemistry and sulphur cycle model to study the impact of terrestrial, i.e. mostly anthropogenic sulphur dioxide (SO 2 ), sources on global distributions of sulphur species in the atmosphere. We briefly address currently available source inventories. It appears that global estimates of natural emissions are associated with uncertainties up to a factor of 2, while anthropogenic emissions have uncertainty ranges of about +/− 30 per cent. Further, some recent improvements in the model descriptions of multiphase chemistry and deposition processes are presented. Dry deposition is modelled consistently with meteorological processes and surface properties. The results indicate that surface removal of SO 2 is less efficient than previously assumed, and that the SO 2 lifetime is thus longer. Coupling of the photochemistry and sulphur chemistry schemes in the model improves the treatment of multiphase processes such as oxidant (hydrogen peroxide) supply in aqueous phase SO 2 oxidation. The results suggest that SO 2 oxidation by ozone (O 3 ) in the aqueous phase is more important than indicated in earlier work. However, it appears that we still overestimate atmospheric SO 2 concentrations near the surface in the relatively polluted Northern Hemisphere. On the other hand, we somewhat underestimate sulphate levels in these regions, which suggests that additional heterogeneous reaction mechanisms, e.g. on aerosols, enhance SO 2 oxidation.

scholarly journals Influence of aromatics on tropospheric gas-phase composition

2020 ◽  
Author(s):  
Domenico Taraborrelli ◽  
David Cabrera-Perez ◽  
Sara Bacer ◽  
Sergey Gromov ◽  
Jos Lelieveld ◽  
...  
Keyword(s):  
East Asia ◽  
Gas Phase ◽  
Atmospheric Chemistry ◽  
General Circulation ◽  
Anthropogenic Activities ◽  
Regional Scale ◽  
Circulation Model ◽  
Significant Loss ◽  
Tropospheric Chemistry ◽  
The Impact

Abstract. Aromatics contribute a significant fraction to organic compounds in the troposphere and are mainly emitted by anthropogenic activities and biomass burning. Their oxidation in lab experiments is known to lead to the formation of ozone and aerosol precursors. However, their overall impact on tropospheric composition is uncertain as it depends on transport, multiphase chemistry, and removal processes of the oxidation intermediates. Representation of aromatics in global atmospheric models has been either neglected or highly simplified. Here, we present an assessment of their impact on the gas-phase chemistry, using the general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). We employ a comprehensive kinetic model to represent the oxidation of the following monocyclic aromatics: benzene, toluene, xylenes, phenol, styrene, ethylbenzene, trimethylbenzenes, benzaldehyde, and lumped higher aromatics that contain more than 9 C atoms. Significant regional changes are identified for several species. For instance, glyoxal increases by 130 % in Europe and 260 % in East Asia, respectively. Large increases in HCHO are also predicted in these regions. In general, the influence of aromatics is particularly evident in areas with high concentrations of NOx, with increases up to 12 % in O3 and 17 % in OH. On a global scale, the estimated net changes are minor when aromatic compounds are included in our model. For instance, the tropospheric burden of CO increases by about 6 %, while the burdens of OH, O3, and NOx (NO + NO2) decrease between 3 % and 9 %. The global mean changes are small, partially because of compensating effects between high- and low-NOx regions. The largest change is predicted for the important aerosol precursor glyoxal, which increases globally by 36 %. In contrast to other studies, the net change in tropospheric ozone is predicted to be negative, −3 % globally. This change is larger in the northern hemisphere where global models usually show positive biases. We find that the reaction with phenoxy radicals is a significant loss for ozone, of the order of 200–300 Tg/yr, which is similar to the estimated ozone loss due to bromine chemistry. Although the net global impact of aromatics is limited, our results indicate that aromatics can strongly influence tropospheric chemistry on a regional scale, most significantly in East Asia. An analysis of the main model uncertainties related to oxidation and emissions suggests that the impact of aromatics may even be significantly larger.

scholarly journals Modeling the impact of heterogeneous reactions of chlorine on summertime nitrate formation in Beijing, China

2018 ◽  
Author(s):  
Xionghui Qiu ◽  
Qi Ying ◽  
Shuxiao Wang ◽  
Lei Duan ◽  
Jian Zhao ◽  
...  
Keyword(s):  
Nitrate Concentration ◽  
Heterogeneous Reaction ◽  
Heterogeneous Reactions ◽  
Sensitivity Analyses ◽  
Uptake Coefficient ◽  
Transport Models ◽  
Nitrate Concentrations ◽  
The Impact ◽  
Beijing China ◽  
Significant Underestimation

Abstract. A comprehensive chlorine heterogeneous chemistry is incorporated into the Community Multiscale Air Quality (CMAQ) model to evaluate the impact of chlorine-related heterogeneous reaction on diurnal and nocturnal nitrate formation and quantify the nitrate formation from gas-to-particle partitioning of HNO3 and from different heterogeneous pathways. The results show that these heterogeneous reactions increase the atmospheric Cl2 and ClNO2 level, leading to an increase of the nitrate concentration by ~ 10 % in the daytime. However, these reactions also lead to a decrease the nocturnal nitrate by ~ 20 %. Sensitivity analyses of uptake coefficients show that the empirical uptake coefficient for the O3 heterogeneous reaction with chlorinated particles may lead to the large uncertainties in the predicted Cl2 and nitrate concentrations. The N2O5 uptake coefficient with particulate Cl− concentration dependence performs better to capture the concentration of ClNO2 and nocturnal nitrate concentration. The reaction rate of OH and NO2 in daytime increases by ~ 15 % when the heterogeneous chlorine chemistry is incorporated, resulting more nitrate formation from HNO3 gas-to-particle partitioning. By contrast, the contribution of the heterogeneous reaction of N2O5 to nitrate concentrations decreases by about 27 % in the nighttime when its reactions with chloriated particles are considered. However, the generated gas-phase ClNO2 from the heterogeneous reaction of N2O5 and chlorine-containing particles further decompose to increase the nitrate by 6 %. In general, this study highlights the potential of significant underestimation of daytime and overestimation of nighttime nitrate concentrations for chemical transport models without proper chlorine chemistry in the gas and particle phases.

scholarly journals Influence of aromatics on tropospheric gas-phase composition

2021 ◽  
Vol 21 (4) ◽  
pp. 2615-2636
Author(s):  
Domenico Taraborrelli ◽  
David Cabrera-Perez ◽  
Sara Bacer ◽  
Sergey Gromov ◽  
Jos Lelieveld ◽  
...  
Keyword(s):  
East Asia ◽  
Gas Phase ◽  
Atmospheric Chemistry ◽  
General Circulation ◽  
Anthropogenic Activities ◽  
Regional Scale ◽  
Circulation Model ◽  
Significant Loss ◽  
Tropospheric Chemistry ◽  
The Impact

Abstract. Aromatics contribute a significant fraction to organic compounds in the troposphere and are mainly emitted by anthropogenic activities and biomass burning. Their oxidation in lab experiments is known to lead to the formation of ozone and aerosol precursors. However, their overall impact on tropospheric composition is uncertain as it depends on transport, multiphase chemistry, and removal processes of the oxidation intermediates. Representation of aromatics in global atmospheric models has been either neglected or highly simplified. Here, we present an assessment of their impact on gas-phase chemistry, using the general circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry). We employ a comprehensive kinetic model to represent the oxidation of the following monocyclic aromatics: benzene, toluene, xylenes, phenol, styrene, ethylbenzene, trimethylbenzenes, benzaldehyde, and lumped higher aromatics that contain more than nine C atoms. Significant regional changes are identified for several species. For instance, glyoxal increases by 130 % in Europe and 260 % in East Asia, respectively. Large increases in HCHO are also predicted in these regions. In general, the influence of aromatics is particularly evident in areas with high concentrations of NOx, with increases up to 12 % in O3 and 17 % in OH. On a global scale, the estimated net changes of trace gas levels are minor when aromatic compounds are included in our model. For instance, the tropospheric burden of CO increases by about 6 %, while the burdens of OH, O3, and NOx (NO+NO2) decrease between 3 % and 9 %. The global mean changes are small, partially because of compensating effects between high- and low-NOx regions. The largest change is predicted for the important aerosol precursor glyoxal, which increases globally by 36 %. In contrast to other studies, the net change in tropospheric ozone is predicted to be negative, −3 % globally. This change is larger in the Northern Hemisphere where global models usually show positive biases. We find that the reaction with phenoxy radicals is a significant loss for ozone, on the order of 200–300 Tg yr−1, which is similar to the estimated ozone loss due to bromine chemistry. Although the net global impact of aromatics is limited, our results indicate that aromatics can strongly influence tropospheric chemistry on a regional scale, most significantly in East Asia. An analysis of the main model uncertainties related to oxidation and emissions suggests that the impact of aromatics may even be significantly larger.

scholarly journals Effects of business-as-usual anthropogenic emissions on air quality

2012 ◽  
Vol 12 (15) ◽  
pp. 6915-6937 ◽  
Author(s):  
A. Pozzer ◽  
P. Zimmermann ◽  
U.M. Doering ◽  
J. van Aardenne ◽  
H. Tost ◽  
...  
Keyword(s):  
Air Pollution ◽  
Air Quality ◽  
East Asia ◽  
South Asia ◽  
Atmospheric Chemistry ◽  
General Circulation ◽  
Circulation Model ◽  
Business As Usual ◽  
The Impact ◽  
Very High

Abstract. The atmospheric chemistry general circulation model EMAC has been used to estimate the impact of anthropogenic emission changes on global and regional air quality in recent and future years (2005, 2010, 2025 and 2050). The emission scenario assumes that population and economic growth largely determine energy and food consumption and consequent pollution sources with the current technologies ("business as usual"). This scenario is chosen to show the effects of not implementing legislation to prevent additional climate change and growing air pollution, other than what is in place for the base year 2005, representing a pessimistic (but plausible) future. By comparing with recent observations, it is shown that the model reproduces the main features of regional air pollution distributions though with some imprecisions inherent to the coarse horizontal resolution (~100 km) and simplified bottom-up emission input. To identify possible future hot spots of poor air quality, a multi pollutant index (MPI), suited for global model output, has been applied. It appears that East and South Asia and the Middle East represent such hotspots due to very high pollutant concentrations, while a general increase of MPIs is observed in all populated regions in the Northern Hemisphere. In East Asia a range of pollutant gases and fine particulate matter (PM2.5) is projected to reach very high levels from 2005 onward, while in South Asia air pollution, including ozone, will grow rapidly towards the middle of the century. Around the Persian Gulf, where natural PM2.5 concentrations are already high (desert dust), ozone levels are expected to increase strongly. The population weighted MPI (PW-MPI), which combines demographic and pollutant concentration projections, shows that a rapidly increasing number of people worldwide will experience reduced air quality during the first half of the 21st century. Following this business as usual scenario, it is projected that air quality for the global average citizen in 2050 would be almost comparable to that for the average citizen in East Asia in the year 2005, which underscores the need to pursue emission reductions.

scholarly journals Effects of business-as-usual anthropogenic emissions on air quality

2012 ◽  
Vol 12 (4) ◽  
pp. 8617-8676
Author(s):  
A. Pozzer ◽  
P. Zimmermann ◽  
U.M. Doering ◽  
J. van Aardenne ◽  
H. Tost ◽  
...  
Keyword(s):  
Air Pollution ◽  
Air Quality ◽  
East Asia ◽  
South Asia ◽  
Atmospheric Chemistry ◽  
General Circulation ◽  
Circulation Model ◽  
Business As Usual ◽  
The Impact ◽  
Very High

Abstract. The atmospheric chemistry general circulation model EMAC has been used to estimate the impact of anthropogenic emission changes on global and regional air quality in recent and future years (2005, 2010, 2025 and 2050). The emission scenario assumes that population and economic growth largely determine energy and food consumption and consequent pollution sources with the current technologies ("business as usual"). This scenario is chosen to show the effects of not implementing legislation to prevent additional climate change and growing air pollution, other than what is in place for the base year 2005, representing a pessimistic (but feasible) future. By comparing with recent observations, it is shown that the model reproduces the main features of regional air pollution distributions though with some imprecisions inherent to the coarse horizontal resolution (~100 km) and simplified bottom-up emission input. To identify possible future hot spots of poor air quality, a multi pollutant index (MPI), suited for global model output, has been applied. It appears that East and South Asia and the Middle East represent such hotspots due to very high pollutant concentrations, although a general increase of MPIs is observed in all populated regions in the Northern Hemisphere. In East Asia a range of pollutant gases and fine particulate matter (PM2.5) is projected to reach very high levels from 2005 onward, while in South Asia air pollution, including ozone, will grow rapidly towards the middle of the century. Around the Arabian Gulf, where natural PM2.5 concentrations are already high (desert dust), ozone levels are expected to increase strongly. The per capita MPI (PCMPI), which combines demographic and pollutants concentrations projections, shows that a rapidly increasing number of people worldwide will experience reduced air quality during the first half of the 21st century. Following the business as usual scenario, it is projected that air quality for the global average citizen in 2050 would be almost comparable to that for the average citizen in the East Asia in the year 2005, which underscores the need to pursue emission reductions.

On the impact of sea ice in a global ocean circulation model

1997 ◽  
Vol 25 ◽  
pp. 111-115 ◽  
Author(s):  
Achim Stössel
Keyword(s):  
Southern Ocean ◽  
Sea Ice ◽  
Ocean Circulation ◽  
General Circulation ◽  
Thermohaline Circulation ◽  
Circulation Model ◽  
Deep Ocean ◽  
Global Ocean ◽  
Convective Activity ◽  
The Impact

This paper investigates the long-term impact of sea ice on global climate using a global sea-ice–ocean general circulation model (OGCM). The sea-ice component involves state-of-the-art dynamics; the ocean component consists of a 3.5° × 3.5° × 11 layer primitive-equation model. Depending on the physical description of sea ice, significant changes are detected in the convective activity, in the hydrographic properties and in the thermohaline circulation of the ocean model. Most of these changes originate in the Southern Ocean, emphasizing the crucial role of sea ice in this marginally stably stratified region of the world's oceans. Specifically, if the effect of brine release is neglected, the deep layers of the Southern Ocean warm up considerably; this is associated with a weakening of the Southern Hemisphere overturning cell. The removal of the commonly used “salinity enhancement” leads to a similar effect. The deep-ocean salinity is almost unaffected in both experiments. Introducing explicit new-ice thickness growth in partially ice-covered gridcells leads to a substantial increase in convective activity, especially in the Southern Ocean, with a concomitant significant cooling and salinification of the deep ocean. Possible mechanisms for the resulting interactions between sea-ice processes and deep-ocean characteristics are suggested.

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