Source apportionment modeling provides valuable information on the contributions of different source sectors and/or source regions to ozone (O3) or fine particulate matter (PM2.5) concentrations. ...This information can be useful in designing air quality management strategies and in understanding the potential benefits of reducing emissions from a particular source category. The Comprehensive Air quality Model with Extensions (CAMx) offers unique source attribution tools, called the Ozone and Particulate Source Apportionment Technology (OSAT/PSAT), which track source contributions. We present results from a CAMx source attribution modeling study for a summer month and a winter month using a recently evaluated European CAMx modeling database developed for Phase 3 of the Air Quality Model Evaluation International Initiative (AQMEII). The contributions of several source sectors (including model boundary conditions of chemical species representing transport of emissions from outside the modeling domain as well as initial conditions of these species) to O3 or PM2.5 concentrations in Europe were calculated using OSAT and PSAT, respectively. A 1-week spin-up period was used to reduce the influence of initial conditions. Evaluation focused on 16 major cities and on identifying source sectors that contributed above 5 %. Boundary conditions have a large impact on summer and winter ozone in Europe and on summer PM2.5, but they are only a minor contributor to winter PM2.5. Biogenic emissions are important for summer ozone and PM2.5. The important anthropogenic sectors for summer ozone are transportation (both on-road and non-road), energy production and conversion, and industry. In two of the 16 cities, solvent and product also contributed above 5 % to summertime ozone. For summertime PM2.5, the important anthropogenic source sectors are energy, transportation, industry, and agriculture. Residential wood combustion is an important anthropogenic sector in winter for PM2.5 over most of Europe, with larger contributions in central and eastern Europe and the Nordic cities. Other anthropogenic sectors with large contributions to wintertime PM2.5 include energy, transportation, and agriculture.
The second phase of the Air Quality Model Evaluation International Initiative (AQMEII) brought together seventeen modeling groups from Europe and North America, running eight operational ...online-coupled air quality models over Europe and North America using common emissions and boundary conditions. The simulated annual, seasonal, continental and sub-regional particulate matter (PM) surface concentrations for the year 2010 have been evaluated against a large observational database from different measurement networks operating in Europe and North America. The results show a systematic underestimation for all models in almost all seasons and sub-regions, with the largest underestimations for the Mediterranean region. The rural PM10 concentrations over Europe are underestimated by all models by up to 66% while the underestimations are much larger for the urban PM10 concentrations (up to 75%). On the other hand, there are overestimations in PM2.5 levels suggesting that the large underestimations in the PM10 levels can be attributed to the natural dust emissions. Over North America, there is a general underestimation in PM10 in all seasons and sub-regions by up to ∼90% due mainly to the underpredictions in soil dust. SO42− levels over EU are underestimated by majority of the models while NO3− levels are largely overestimated, particularly in east and south Europe. NH4+ levels are also underestimated largely in south Europe. SO4 levels over North America are particularly overestimated over the western US that is characterized by large anthropogenic emissions while the eastern USA is characterized by underestimated SO4 levels by the majority of the models. Daytime AOD levels at 555 nm is simulated within the 50% error range over both continents with differences attributed to differences in concentrations of the relevant species as well as in approaches in estimating the AOD. Results show that the simulated dry deposition can lead to substantial differences among the models. Overall, the results show that representation of dust and sea-salt emissions can largely impact the simulated PM concentrations and that there are still major challenges and uncertainties in simulating the PM levels.
•Seventeen modeling groups from EU and NA simulated PM for 2010 under AQMEII phase 2.•A general model underestimation of surface PM over both continents up to 80%.•Natural PM emissions may lead to large underestimations in simulated PM10.•Dry deposition can introduce large differences among models.
Recent observation and modeling-based studies have shown how air quality has been positively affected by the containment measures enforced due to the COVID-19 outbreak. This work aims to analyze ...Lombardy’s NO2 atmospheric concentration during the spring lockdown. The region of Lombardy is known for having the largest number of residents in Italy and high levels of pollution. It is also the region where the first European confinement measures were imposed by the Italian government. The modeling suite composed of CAMx (Comprehensive Air Quality Model with Extensions) and WRF (Weather Research and Forecasting model) provides the setting to compare the atmospheric NO2 concentration from mid-February to the end of March with a business as usual situation. The main interest in this work is to investigate the response of NO2 atmospheric concentration to increasingly reduced road traffic. We can simulate, for the first time, a real circumstance of progressively reduced mobility, as well as validating it with measured air quality data. Focusing on the city of Milan, we found that the decrease in NO2 concentration reflects progressively reduced traffic contraction. In the case of a large traffic abatement (71%), the concentration level is reduced by one third. We also find that industrial activities have a relevant impact on NO2 atmospheric concentration, especially in the provinces of Brescia and Bergamo. This study provides an overview of how incisive policies must be implemented to achieve the set environmental targets and protect human health.
Air quality modeling at the very local scale within an urban area is performed through a hybrid modeling system (HMS) that combines the CAMx Eulerian model the with AUSTAL2000 Lagrangian model. The ...enhancements obtained by means of the HMS in the reconstruction of the spatial distribution of fine particles (PM2.5) and elemental carbon (EC) concentration are presented for the case-study of Milan city center in Northern Italy. Modeling results are reported for three receptors (a green area, a residential and shopping area, and a congested crossroad on the inner ring road of the city center) selected in order to represent urban sites characterized by both different features in terms of the surrounding built environment and by different exposure to local emission sources. The peculiarity of the three receptors is further highlighted by source apportionment analysis, developed not only with respect to the kind of emission sources but also to the geographical location of the sources within the whole Northern Italy computational domain. Results show that the outcome of the Eulerian model at the local scale is only representative of a background level, similar to the Lagrangian model’s outcome for the green area receptor, but fails to reproduce concentration gradients and hot-spots, driven by local sources’ emissions.
The reliability of the national power grid is a key issue in modern society. Atmospheric aerosols are the main cause of the reduction in the performance of insulators and the increase in the ...possibility of flashovers, resulting in power line failures. Under high ambient humidity, the water-soluble compounds of atmospheric aerosols collected on the insulators’ surface can dissociate in ions and form a conductive layer, which may lead to flashover events. With a view to investigating the processes that drive these phenomena, the chemical composition of aerosol deposits on insulators in Italy was determined by ion chromatography analysis and thermos-optical and X-ray techniques. In addition, a synthetic aerosol with the same analyzed chemical composition was generated in a laboratory and deposited on PTFE filters and glass specimens allowing us to determine the deliquescence and crystallization relative humidity and the conductive effect in an aerosol exposure chamber. The results evidenced the presence of a hazardous inorganic ion layer, which generates a sharp phase transition of the aerosol deposit as a function of the ambient relative humidity; this layer poses a dangerous threat to the reliability of the power grid, increasing the probability of flashover events where the conductive layer facilitates the flow of electrical current across the insulator surface, potentially causing power outages or damage to the power lines.
A new sensitivity analysis with the Comprehensive Air Quality Model with Extensions (CAMx) using a traditional two-product scheme (SOAP) and the newer Volatility Basis Set (VBS) algorithm for organic ...aerosol (OA) calculations is presented. The sensitivity simulations include the default versions of the SOAP and VBS schemes, as well as new parametrizations for the VBS scheme to calculate emissions and volatility distributions of semi- and intermediate-volatile organic compounds. The focus of the simulations is the summer season (May to July 2013), in order to quantify the sensitivity of the model in a period with relatively large photochemical activity. In addition to the model sensitivity, we validate the results with ad hoc OA measurements obtained from aerosol mass spectrometers at two monitoring sites. Unlike winter cases previously published, the comparison with experimental data showed limited sensitivity to total OA amount, with an estimated increase in OA concentrations limited to a few tenths of µg m−3, for both the primary and secondary components. We show that the lack of pronounced sensitivity is related to the effect of the new parametrizations on different emissions sectors. Furthermore, the minor sensitivity to the new parametrizations could be related to the greater partitioning of OA towards the gaseous phase in the summer period, thus reducing the organic fraction in the aerosol phase.
This study presents a high–resolution (5 km) set of new simulations performed with CAMx v6.40 over the Po Valley area (Northern Italy), aimed to enhance organic aerosol (OA) levels prediction and to ...gain insight into the sensitivity of CAMx to different uncertain features of the input setup. In particular, we mainly investigated the role of (i) volatility distributions of organic emissions, (ii) parametrizations of semi– and intermediate–volatile organic compounds (S/IVOC) emissions and (iii) different aging schemes, by exploiting the latest experimental information available in the recent scientific literature. Model results were validated against two OA–specific datasets, available for both an urban site (Bologna, February 2013) and a rural one (Ispra, March 2013).
We found out a remarkable performance enhancement of modelled OA levels when applying revisions in S/IVOC emission parametrizations together with the new volatility distributions, at both the validation sites. This performance enhancement is associated with a very significant improvement in secondary organic aerosol (SOA) prediction, mainly due to revised IVOC emissions. At Bologna urban site, mean fractional bias (MFB) of OA ranged from −80.1% in the worst run to −10.1% in the best one and index of agreement (IOA) from 0.52 to 0.75. Notable improvements but overall poorer metrics were found for Ispra site, where MFB ranges from −84.2% to −35% and IOA from 0.45 to 0.50. These findings indicate that organic matter in the semi– and intermediate–volatile range are most likely underestimated in official emission inventories for each main source category (i.e. biomass burning, diesel and gasoline vehicles exhaust).
Finally, model results did not show a very pronounced sensitivity to aging processes, due to the low photochemical activity typically observed during winter–time. However, we give evidence that enabling aging processes for biomass burning related SOA, which is by default disabled in CAMx v6.40, can help in closing the gap between modelled and observed SOA concentrations.
•Latest experimental studies about emissions of organic matter implemented in CAMx.•Remarkable improvement on modelled organic aerosol levels.•S/IVOC emission revisions appear to be the key factor for such improvement.•Enabling aging processes for biomass burning SOA enhances the performance of the model.•VBS provides a better reconstruction of POA and SOA relative contribution to the total.
The impact of air pollution on human health and the associated external costs in Europe and the United States (US) for the year 2010 are modeled by a multi-model ensemble of regional models in the ...frame of the third phase of the Air Quality Modelling Evaluation International Initiative (AQMEII3). The modeled surface concentrations of O
, CO, SO
and PM
are used as input to the Economic Valuation of Air Pollution (EVA) system to calculate the resulting health impacts and the associated external costs from each individual model. Along with a base case simulation, additional runs were performed introducing 20 % anthropogenic emission reductions both globally and regionally in Europe, North America and east Asia, as defined by the second phase of the Task Force on Hemispheric Transport of Air Pollution (TF-HTAP2). Health impacts estimated by using concentration inputs from different chemistry-transport models (CTMs) to the EVA system can vary up to a factor of 3 in Europe (12 models) and the United States (3 models). In Europe, the multi-model mean total number of premature deaths (acute and chronic) is calculated to be 414 000, while in the US, it is estimated to be 160 000, in agreement with previous global and regional studies. The economic valuation of these health impacts is calculated to be EUR 300 billion and 145 billion in Europe and the US, respectively. A subset of models that produce the smallest error compared to the surface observations at each time step against an all-model mean ensemble results in increase of health impacts by up to 30 % in Europe, while in the US, the optimal ensemble mean led to a decrease in the calculated health impacts by ~ 11 %. A total of 54 000 and 27 500 premature deaths can be avoided by a 20 % reduction of global anthropogenic emissions in Europe and the US, respectively. A 20 % reduction of North American anthropogenic emissions avoids a total of ~ 1000 premature deaths in Europe and 25 000 total premature deaths in the US. A 20 % decrease of anthropogenic emissions within the European source region avoids a total of 47 000 premature deaths in Europe. Reducing the east Asian anthropogenic emissions by 20 % avoids ~ 2000 total premature deaths in the US. These results show that the domestic anthropogenic emissions make the largest impacts on premature deaths on a continental scale, while foreign sources make a minor contribution to adverse impacts of air pollution.
As a contribution to phase2 of the Air Quality Model Evaluation International Initiative (AQMEII), eight different simulations for the year 2010 were performed with WRF-Chem for the European domain. ...The four simulations using RADM2 gas-phase chemistry and the MADE/SORGAM aerosol module are analyzed in this paper. The simulations included different degrees of aerosol–meteorology feedback, ranging from no aerosol effects at all to the inclusion of the aerosol direct radiative effect as well as aerosol cloud interactions and the aerosol indirect effect. In addition, a modification of the RADM2 gas phase chemistry solver was tested. The yearly simulations allow characterizing the average impact of the consideration of feedback effects on meteorology and pollutant concentrations and an analysis of the seasonality. Pronounced feedback effects were found for the summer 2010 Russian wildfire episode, where the direct aerosol effect lowered the seasonal mean solar radiation by 20 W m−3 and seasonal mean temperature by 0.25°. This might be considered as a lower limit as it must be taken into account that aerosol concentrations were generally underestimated by up to 50%. The high aerosol concentrations from the wildfires resulted in a 10%–30% decreased precipitation over Russia when aerosol cloud interactions were taken into account. The most pronounced and persistent feedback due to the indirect aerosol effect was found for regions with very low aerosol concentrations like the Atlantic and Northern Europe. The low aerosol concentrations in this area result in very low cloud droplet numbers between 5 and 100 droplets cm−1 and a 50–70% lower cloud liquid water path. This leads to an increase in the downward solar radiation by almost 50%. Over Northern Scandinavia, this results in almost one degree higher mean temperatures during summer. In winter, the decreased liquid water path resulted in increased long-wave cooling and a decrease of the mean temperature by almost the same amount. Precipitation over the Atlantic Ocean was found to be enhanced by up to 30% when aerosol cloud interactions were taken into account. The inclusion of aerosol cloud interactions can reduce the bias or improve correlations of simulated precipitation for some episodes and regions. However, the domain and time averaged performance statistics do not indicate a general improvement when aerosol feedbacks are taken into account. Except for conditions with either very low or very high aerosol concentrations, the impact of aerosol feedbacks on pollutant distributions was found to be smaller than the effect of the choice of the chemistry module or wet deposition implementation.
•We compare four WRF-Chem simulations which contributed to AQMEII phase2.•Simulations include different degrees of aerosol–radiation feedback and aerosol cloud interactions.•Lower solar radiation, temperature, PBL height, and ozone with direct aerosol effect.•With aerosol cloud interactions higher solar radiation for clean conditions.•Neutral on average performance except for very low aerosol concentrations.
The second phase of the Air Quality Model Evaluation International Initiative (AQMEII) brought together sixteen modeling groups from Europe and North America, running eight operational online-coupled ...air quality models over Europe and North America on common emissions and boundary conditions. With the advent of online-coupled models providing new capability to quantify the effects of feedback processes, the main aim of this study is to compare the response of coupled air quality models to simulate levels of O3 over the two continental regions. The simulated annual, seasonal, continental and sub-regional ozone surface concentrations and vertical profiles for the year 2010 have been evaluated against a large observational database from different measurement networks operating in Europe and North America. Results show a general model underestimation of the annual surface ozone levels over both continents reaching up to 18% over Europe and 22% over North America. The observed temporal variations are successfully reproduced with correlation coefficients larger than 0.8. Results clearly show that the simulated levels highly depend on the meteorological and chemical configurations used in the models, even within the same modeling system. The seasonal and sub-regional analyses show the models' tendency to overestimate surface ozone in all regions during autumn and underestimate in winter. Boundary conditions strongly influence ozone predictions especially during winter and autumn, whereas during summer local production dominates over regional transport. Daily maximum 8-h averaged surface ozone levels below 50–60 μg m−3 are overestimated by all models over both continents while levels over 120–140 μg m−3 are underestimated, suggesting that models have a tendency to severely under-predict high O3 values that are of concern for air quality forecast and control policy applications.
•Sixteen modeling groups from EU and NA simulated O3 for 2010 under AQMEII phase 2.•A general model underestimation of surface O3 over both continents up to 22%.•Models tend to over/under estimate surface O3 in all regions during autumn/winter.•Boundary conditions influence O3 predictions especially during winter and autumn.•Models tend to under-predict high O3 values that are of concern for policy.
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