Rural Background Stations Research Articles

Dynamic evaluation of modeled ozone concentrations in Germany with four chemistry transport models

Simulating the ozone variability at regional scales using chemistry transport models (CTMs) remains a challenge. We designed a multi-model intercomparison to evaluate, for the first time, four regional CTMs on a national scale for Germany. Simulations were conducted with LOTOS-EUROS, REM-CALGRID, COSMO-MUSCAT and WRF-Chem for January 1st to December 31st, 2019, using prescribed emission information. In general, all models show good performance in the operational evaluation with average temporal correlations of MDA8 O3 in the range of 0.77–0.87 and RMSE values between 16.3 μg m−3 and 20.6 μg m−3. On average, better models' skill has been observed for rural background stations than for the urban background stations as well as for springtime compared to summertime. Our study confirms that the ensemble mean provides a better model-measurement agreement than individual models. All models capture the larger local photochemical production in summer compared to springtime and observed differences between the urban and the rural background. We introduce a new indicator to evaluate the dynamic response of ozone to temperature. During summertime a large ensemble spread in the ozone sensitivities to temperature is found with (on average) an underestimation of the ozone sensitivity to temperature, which can be linked to a systematic underestimation of mid-level ozone concentrations. During springtime we observed an ozone episode that is not covered by the models which is likely due to deficiencies in the representation of background ozone in the models. We recommend to focus on a diagnostic evaluation aimed at the model descriptions for biogenic emissions and dry deposition as a follow up and to repeat the operational and dynamic analysis for longer timeframes.

Identification of volatile organic compounds and their sources driving ozone and secondary organic aerosol formation in NE Spain

Volatile organic compounds (VOCs) play a crucial role in the formation of ozone (O3) and secondary organic aerosol (SOA). We conducted measurements of VOC ambient mixing ratios during both summer and winter at two stations: a Barcelona urban background station (BCN) and the Montseny rural background station (MSY). Subsequently, we employed positive matrix factorization (PMF) to analyze the VOC mixing ratios and identify their sources. Our analysis revealed five common sources: anthropogenic I (traffic & industries); anthropogenic II (traffic & biomass burning); isoprene oxidation; monoterpenes; long-lifetime VOCs. To assess the impact of these VOCs on the formation of secondary pollutants, we calculated the ozone formation potential (OFP) and secondary organic aerosol formation potential (SOAP) associated with each VOC. In conclusion, our study provides insights into the sources of VOCs and their contributions to the formation of ozone and SOA in NE Spain. The OFP was primarily influenced by anthropogenic aromatic compounds from the traffic & industries source at BCN (38–49 %) and during winter at MSY (34 %). In contrast, the summer OFP at MSY was primarily driven by biogenic contributions from monoterpenes and isoprene oxidation products (45 %). Acetaldehyde (10–35 %) and methanol (13–14 %) also made significant OFP contributions at both stations. Anthropogenic aromatic compounds originating from traffic, industries, and biomass burning played a dominant role (88–93 %) in SOA formation at both stations during both seasons. The only exception was during the summer at MSY, where monoterpenes became the primary driver of SOA formation (41 %). These findings emphasize the importance of considering both anthropogenic and biogenic VOCs in air quality management strategies.

A 1-year aerosol chemical speciation monitor (ACSM) source analysis of organic aerosol particle contributions from anthropogenic sources after long-range transport at the TROPOS research station Melpitz

Abstract. Atmospheric aerosol particles are a complex combination of primary emitted sources (biogenic and anthropogenic) and secondary aerosol resulting from aging processes such as condensation, coagulation, and cloud processing. To better understand their sources, investigations have been focused on urban areas in the past, whereas rural-background stations are normally less impacted by surrounding anthropogenic sources. Therefore, they are predisposed for studying the impact of long-range transport of anthropogenic aerosols. Here, the chemical composition and organic aerosol (OA) sources of submicron aerosol particles measured by an aerosol chemical speciation monitor (ACSM) and a multi-angle absorption photometer (MAAP) were investigated at Melpitz from September 2016 to August 2017. The location of the station at the frontier between western and eastern Europe makes it the ideal place to investigate the impact of long-range transport over Europe. Indeed, the station is under the influence of less polluted air masses from westerly directions and more polluted continental air masses from eastern Europe. The OA dominated the submicron particle mass concentration and showed strong seasonal variability ranging from 39 % (in winter) to 58 % (in summer). It was followed by sulfate (15 % and 20 %) and nitrate (24 % and 11 %). The OA source identification was performed using the rolling positive matrix factorization (PMF) approach to account for the potential temporal changes in the source profile. It was possible to split OA into five factors with a distinct temporal variability and mass spectral signature. Three were associated with anthropogenic primary OA (POA) sources: hydrocarbon-like OA (HOA; 5.2 % of OA mass in winter and 6.8 % in summer), biomass burning OA (BBOA; 10.6 % and 6.1 %) and coal combustion OA (CCOA; 23 % and 8.7 %). Another two are secondary and processed oxygenated OA (OOA) sources: less oxidized OOA (LO-OOA; 28.4 % and 36.7 %) and more oxidized OOA (MO-OOA; 32.8 % and 41.8 %). Since equivalent black carbon (eBC) was clearly associated with the identified POA factors (sum of HOA, BBOA, and CCOA; R2= 0. 87), eBC's contribution to each of the POA factors was achieved using a multilinear regression model. Consequently, CCOA represented the main anthropogenic sources of carbonaceous aerosol (sum of OA and eBC) not only during winter (56 % of POA in winter) but also in summer (13 % of POA in summer), followed by BBOA (29 % and 69 % of POA in winter and summer, respectively) and HOA (15 % and 18 % of POA in winter and summer, respectively). A seasonal air mass cluster analysis was used to understand the geographical origins of the different aerosol types and showed that during both winter and summer time, PM1 (PM with an aerodynamic diameter smaller than 1 µm) air masses with eastern influence were always associated with the highest mass concentration and the highest coal combustion fraction. Since during wintertime CCOA is a combination of domestic heating and power plant emissions, the summer contribution of CCOA emphasizes the critical importance of coal power plant emissions to rural-background aerosols and its impact on air quality, through long-range transportation.

Ionic composition of six-year daily precipitation samples collected at JRC-Ispra (Italy) in relation to synoptic patterns and air mass origin

A six-year dataset of daily precipitation samples collected and analyzed at the rural background station of Joint Research Center (JRC) at Ispra (Italy), was studied in conjunction with synoptic patterns and Concentration Weighted Trajectory (CWT) model in order to identify atmospheric mechanisms and transport pathways affecting the concentrations of eight major inorganic ions: NO3−, Cl−, Na+, Mg2+, Ca2+, SO42−, NH4+ and K+. A Principal Component Analysis (PCA) distributed the studied constituents to three categories reflecting major emission sources: a) Anthropogenic b) Sea salt and c) Crustal. The concentrations of all ions in precipitation samples were negatively correlated with precipitation amounts, however the negative correlations were more enhanced for species having a mainly anthropogenic origin (NO3−, SO42−, NH4+ and K+). The anthropogenic constituents were transported mainly from continental Europe, while the primary role of emissions in the industrialized Po Valley was highlighted from the impact of Eastern airflows on NO3−, SO42−, NH4+ and K+ levels. In addition, a secondary Saharan dust source for SO42− was verified. Sea salt species (Cl−, Na+ and Mg2+) were originated from the Mediterranean Sea, the North Sea, the Baltic Sea, and possibly from the Atlantic through France, while Saharan dust intrusions clearly enhanced the levels of crustal constituents (Ca2+ and Mg2+). The elaboration of a multi-year precipitation dataset for the first time with CWT model, provided new insights regarding the emission sources and transport mechanisms affecting the ionic composition of precipitation samples collected at JRC-Ispra.

Links between the concentrations of gaseous pollutants measured in different regions of Estonia.

The factors that determine the concentrations of air pollutants (NO, NO2, SO2, O3), measured in 8 monitoring stations (4 rural background, 3 urban, and 1 industrial) in Estonia, are studied applying the factor analysis. The factor analysis reveals remarkable impact of COVID-19 lockdown, effects caused by dramatic decrease in oil-shale based energy production in Estonia provoked by new socio-economic conditions such as elevated price for CO2 emission quota, differences between rural and urban stations, maritime-continental difference for NO2 and ozone, and specific industrial impact in case of SO2. The multiple regression analysis to predict the ozone concentration in one rural background station at Tahkuse was performed, based on the ozone concentrations measured in other stations and the concentrations of NO, NO2, and CO2, recorded in the same station. It was found that the ozone concentration at Tahkuse is rather well predictable (determination coefficient, i.e., correlation coefficient squared, R2 = 0.714), using only the concentrations from another rural station at Saarejärve that is about 110 km away from Tahkuse. Adding all the available data into the list of regression analysis arguments, the model predictability is improved moderately (determination coefficient R2 = 0.795). Large model residuals above all tend to occur with the values measured and predicted at summer nights. Surprisingly, neither NO nor NO2 concentration measured in the Tahkuse station did appear a good predictor for ozone (R2 = 0.02 and 0.05, respectively), possibly long-range transport of ozone (that has also experienced NO and/or NO2 influence during transport) overrides the local effects of NO and/or NO2.

Comparison of S5P/TROPOMI Inferred NO2 Surface Concentrations with In Situ Measurements over Central Europe

The aim of this paper is to evaluate the surface concentration of nitrogen dioxide (NO2) inferred from the Sentinel-5 Precursor Tropospheric Monitoring Instrument (S5P/TROPOMI) NO2 tropospheric column densities over Central Europe for two time periods, summer 2019 and winter 2019–2020. Simulations of the NO2 tropospheric vertical column densities and surface concentrations from the Long-Term Ozone Simulation–European Operational Smog (LOTOS-EUROS) chemical transport model are also applied in the methodology. More than two hundred in situ air quality monitoring stations, reporting to the European Environment Agency (EEA) air quality database, are used to carry out comparisons with the model simulations and the spaceborne inferred surface concentrations. Stations are separated into seven types (urban traffic, suburban traffic, urban background, suburban background, rural background, suburban industrial and rural industrial) in order to examine the strengths and shortcomings of the different air quality markers, namely the NO2 vertical column densities and NO2 surface concentrations. S5P/TROPOMI NO2 surface concentrations are inferred by multiplying the fraction of the satellite and model NO2 vertical column densities with the model surface concentrations. The estimated inferred TROPOMI NO2 surface concentrations are examined further with the altering of three influencing factors: the model vertical leveling scheme, the versions of the TROPOMI NO2 data and the air mass factors applied to the satellite and model NO2 vertical column densities. Overall, the inferred TROPOMI NO2 surface concentrations show a better correlation with the in situ measurements for both time periods and all station types, especially for the industrial stations (R > 0.6) in winter. The calculated correlation for background stations is moderate for both periods (R~0.5 in summer and R > 0.5 in winter), whereas for traffic stations it improves in the winter (from 0.20 to 0.50). After the implementation of the air mass factors from the local model, the bias is significantly reduced for most of the station types, especially in winter for the background stations, ranging from +0.49% for the urban background to +10.37% for the rural background stations. The mean relative bias in winter between the inferred S5P/TROPOMI NO2 surface concentrations and the ground-based measurements for industrial stations is about −15%, whereas for traffic urban stations it is approximately −25%. In summer, biases are generally higher for all station types, especially for the traffic stations (~−75%), ranging from −54% to −30% for the background and industrial stations.

Modelling ultrafine particle number concentrations at address resolution in Denmark from 1979 to 2018 - Part 2: Local and street scale modelling and evaluation

Modelling of ambient particle number concentrations (PNC) has been implemented in the Danish air quality modelling system DEHM/UBM/AirGIS and evaluated with long-term measurements. We implemented particle dynamical processes in the regional scale model DEHM using the M7 aerosol dynamics module (presented in the accompanying article by Frohn et al., 2021), and we developed models for PNC at the local scale (UBM) and street scale (OSPM), in a first approximation without including the particle dynamics as presented in this article.Outdoor concentration estimates are provided at the front door of all residential address locations in Denmark for the past 40 years (1979–2018) with a spatial resolution of 1 km × 1 km taking all emission sectors in Denmark into account and additionally at the street location, with significant traffic (>500 vehicles/day).We evaluated our model with up to 18-year long measurement time series of particle number size distributions (PNSD) at Danish street, urban and rural background stations. Two particle size ranges were used for evaluation: PNC>10 (count of particles with diameter larger than 10 nm) and PNC30_250 (diameter range 30–250 nm), in order to exclude nucleation events from the measurements and to obtain a consistent long-term measured time series.When comparing our model estimates with PNC30_250 measurements, we obtain Pearson correlation coefficients (Rp) in the range 0.39–0.95 depending on station location (street, urban background, rural) and averaging time (hour, day, month, year). The highest correlations were found for yearly averages at a monitoring station located at a street with dense traffic (Rp = 0.95) whereas shorter time averages and comparisons with monitoring stations at urban and rural background locations provided lower correlations. The model performance for PNC in terms of correlation coefficients with respect to measurements is comparable to the performance for other pollutants such as NOX, PM2.5 and better than the performance for PM10.The model generally overestimated the observed concentrations, Normalized Mean Bias (NMB) was in the range 6%–190% compared to PNC>10 and 90%–290% compared to PNC30_250. These relatively high NMBs are probably caused by uncertainties in the modelling process, especially the estimation of particle number emissions, which largely determine the ambient concentrations of PNC. Furthermore, uncertainties might as well originate from the complexity of modelling particle dynamical processes accurately and the great challenges in performing long-term PNC measurements.The presented model can estimate PNC at all Danish addresses over the last 40 years with a 1-h time resolution. The data seem to provide a good indication of the relative differences in PNC at Danish addresses.

Air quality assessment in three East African cities using calibrated low-cost sensors with a focus on road-based hotspots

Poor air quality is a development challenge. Urbanization and industrial development along with increased populations have brought clear socio-economic benefits to Low-and Middle-Income Countries (LMICs) but can also bring disadvantages such as decreasing air quality. A lack of reliable air quality data in East African cities makes it difficult to understand air pollution exposure and to predict future air quality trends. This work documents urban air quality and air pollution exposure in the capital cities of Kampala (Uganda), Addis Ababa (Ethiopia) and Nairobi (Kenya). We build a situational awareness of air pollution through repeated static and dynamic mobile monitoring in a range of urban locations, including urban background, roadside (pavement and building), rural background, and bus station sites, alongside vehicle-based measurements including buses and motorcycle taxis. Data suggest that the measured particulate matter mass concentrations (PM2.5, PM10) in all studied cities was at high concentrations, and often hazardous to human health, as defined by WHO air quality guidelines. Overall, the poorest air quality was observed in Kampala, where mean daily PM2.5 and PM10 concentrations were significantly above the WHO limits at urban background locations by 122% and 69% and at roadside locations by 193% and 215%, respectively. Traffic is clearly a major contributor to East African urban air pollution; monitoring in Kampala and Addis Ababa, on motorcycle taxis, in buses and at bus stations indicated that drivers and commuters were exposed to poor air quality throughout their commute. Road-related air pollution can also impact indoor locations near roads. Using one exemplar building located within Nairobi’s Central Business District, it is shown that measured outdoor PM concentrations significantly correlate with the indoor air quality (r = 0.84). This link between roadside emissions and indoor air pollution within buildings located close to the road should be explored more fully. This study, through a series of case studies, provides clear evidence that roads and traffic need to be a focus for mitigation strategies to reduce air pollution exposure in East African cities.

Compositional changes of PM2.5 in NE Spain during 2009–2018: A trend analysis of the chemical composition and source apportionment

In this work, time-series analyses of the chemical composition and source contributions of PM2.5 from an urban background station in Barcelona (BCN) and a rural background station in Montseny (MSY) in northeastern Spain from 2009 to 2018 were investigated and compared. A multisite positive matrix factorization analysis was used to compare the source contributions between the two stations, while the trends for both the chemical species and source contributions were studied using the Theil–Sen trend estimator. Between 2009 and 2018, both stations showed a statistically significant decrease in PM2.5 concentrations, which was driven by the downward trends of levels of chemical species and anthropogenic source contributions, mainly from heavy oil combustion, mixed combustion, industry, and secondary sulfate. These source contributions showed a continuous decrease over the study period, signifying the continuing success of mitigation strategies, although the trends of heavy oil combustion and secondary sulfate have flattened since 2016. Secondary nitrate also followed a significant decreasing trend in BCN, while secondary organic aerosols (SOA) very slightly decreased in MSY. The observed decreasing trends, in combination with the absence of a trend for the organic aerosols (OA) at both stations, resulted in an increase in the relative proportion of OA in PM2.5 by 12% in BCN and 9% in MSY, mostly from SOA, which increased by 7% in BCN and 4% in MSY. Thus, at the end of the study period, OA accounted for 40% and 50% of the annual mean PM2.5 at BCN and MSY, respectively. This might have relevant implications for air quality policies aiming at abating PM2.5 in the study region and for possible changes in toxicity of PM2.5 due to marked changes in composition and source apportionment.

Mass absorption cross-section and absorption enhancement from long term black and elemental carbon measurements: A rural background station in Central Europe

Black carbon (BC) is a dominant aerosol light absorber, and its brown carbon (BrC) coating can enhance absorption and lead to uncertainties concerning the radiative forcing estimation. This study investigates the mass absorption cross-section of equivalent BC (MACeBC) during a long-term field measurement (2013–2017) at a rural Central European site. The MAC enhancement factor (Eabs) and the contribution of BrC coatings to the absorption coefficient (Babs) were estimated by combining different approaches. The annual mean Babs and MACeBC values decreased slightly over the measurement period associated with change in the submicron aerosol size distribution. Regardless of the wavelength, Babs exhibited clear seasonal and diurnal variations, with higher values in winter when a higher absorption Ångström exponent (1.4) was observed due to the local biomass burning (BB). In contrast, MACeBC did not have a distinct temporal trend at 600 nm (7.84 ± 2.79 m2 g−1), while it showed a seasonal trend at 370 nm with higher values in winter (15.64 ± 4.77 m2 g−1). During this season, Eabs_660 was 1.18 ± 0.27 and did not exhibit any clear wavelength dependence, despite the influence of BB. During the study period, BrC-attributed absorption was observed in 31% of the samples, with a contribution of up to 40% of total Babs. In summer, the Eabs_660 increased to 1.59 ± 0.60, when a larger BC coating could be formed by secondary aerosol fractions. During this season, MACeBC_660 and Eabs_660 showed comparable source profiles that were mainly associated with aged air masses over central Europe, thereby supporting the fact that characteristics of coating materials formed during atmospheric aging are a major factor driving the MACeBC_660 measured at the regional background site. Further field investigations of the composition of BC coatings would help to better understand and estimate uncertainties related to the radiative effect of aerosols.

Source Apportionment and Toxicity of PM in Urban, Sub-Urban, and Rural Air Quality Network Stations in Catalonia

Air quality indicators, i.e., PM10, NO2, O3, benzo[a]pyrene, and several organic tracer compounds were evaluated in an urban traffic station, a sub-urban background station, and a rural background station of the air quality network in Catalonia (Spain) from summer to winter 2019. The main sources that contribute to the organic aerosol and PM toxicity were determined. Traffic-related air pollution dominated the air quality in the urban traffic station, while biomass burning in winter and secondary organic aerosol (SOA) in summer impact the air quality in the sub-urban and rural background stations. Health risk assessment for chronic exposure over the past decade, using WHO air quality standards, showed that NO2, PM10 and benzo[a]pyrene from traffic emissions pose an unacceptable risk to the human population in the urban traffic station. PM10 and benzo[a]pyrene from biomass burning were unacceptably high in the sub-urban and rural background stations. Toxicity tests of the PM extracts with epithelial lung cells showed higher toxicity in wintertime samples in the sub-urban and rural stations, compared to the urban traffic station. These results require different mitigation strategies for urban and rural sites in order to improve the air quality. In urban areas, traffic emissions are still dominating the air quality, despite improvements in the last years, and may directly be responsible for part of the SOA and O3 levels in sub-urban and rural areas. In these later areas, air pollution from local biomass burning emissions are dominating the air quality, essentially in the colder period of the year.

Nitrogen dioxide reductions from satellite and surface observations during COVID-19 mitigation in Rome (Italy)

Lockdown restrictions were implemented in Italy from 10 March 2020 to contain the COVID-19 pandemic. Our study aims to evaluate air pollution changes, with focus on nitrogen dioxide (NO2), before and during the lockdown in Rome and in the surroundings. Significant NO2 declines were observed during the COVID-19 pandemic with reductions of − 50%, − 34%, and − 20% at urban traffic, urban background, and rural background stations, respectively. Tropospheric NO2 vertical column density (VCD) from the TROPOspheric Monitoring Instrument (TROPOMI) was used to evaluate the spatial-temporal variations of the NO2 before and during the lockdown for the entire area where the surface stations are located. The evaluation is concerned with the pixels including one or more air quality stations to explore the capability of the unprecedented high spatial resolution to monitor urban and rural sites from space with relation to the surface measurements. Good agreement between surface concentration and TROPOMI VCD was obtained in Rome (R = 0.64 in 2019, R = 0.77 in 2020) and in rural sites (R = 0.71 in 2019). Inversely, a slight correlation (R = 0.20) was observed in rural areas during the lockdown due to very low levels of NO2. Finally, the TROPOMI VCD showed a sharp decline in NO2, larger in urban (− 43%) than in rural sites (− 17%) as retrieved with the concurrent surface measurements averaging all the traffic and urban background (− 44%) and all the rural background stations (− 20%). These results suggest air pollution improvement in Rome gained from implementing lockdown restrictions.

Hidden black carbon air pollution in hilly rural areas—a case study of Dinaric depression

Air pollution is not an exclusively urban problem as wood burning is a widespread practice in rural areas. As we lack information on the air quality situation in rural mountainous regions, our aim is to examine equivalent black carbon (eBC) pollution in a typical rural karst area in the settlement of Loški Potok (Slovenia). eBC mass concentrations were measured by Aethalometer (AE-33) at two sites in Retje karst depression. The rural village station was located at the bottom of the karst depression whereas the rural background station was positioned at the top of the hill. We show the diurnal variation of equivalent black carbon mass concentrations for different seasons. In the populated karst depression, the major source of eBC pollution are households using wood as a heating fuel reaching the highest mass concentrations in winter. Diurnal pattern of eBC from biomass burning and traffic differ due to different source activity and it is influenced by typical formation of a cold air pool from late afternoon until late morning, restricting the dispersion of local emissions. The large difference in mass concentrations between the lowest part of the village (rural station) and the top of the hill (rural background station) indicates that in a vertically stratified and stable atmosphere local sources of black carbon have a major impact on air quality conditions in the area studied. Since in Alpine and Dinaric regions there are many similar inhabited areas, we can expect similar air quality conditions also in other rural hilly areas with limited self-cleaning air capacity.

Aerosol pollution maps and trends over Germany with hourly data at four rural background stations from 2009 to 2018

Abstract. A total of 10 years of hourly aerosol and gas data at four rural German stations have been combined with hourly back trajectories to the stations and inventories of the European Emissions Database for Global Atmospheric Research (EDGAR), yielding pollution maps over Germany of PM10, particle number concentrations, and equivalent black carbon (eBC). The maps reflect aerosol emissions modified with atmospheric processes during transport between sources and receptor sites. Compared to emission maps, strong western European emission centers do not dominate the downwind concentrations because their emissions are reduced by atmospheric processes on the way to the receptor area. PM10, eBC, and to some extent also particle number concentrations are rather controlled by emissions from southeastern Europe from which pollution transport often occurs under drier conditions. Newly formed particles are found in air masses from a broad sector reaching from southern Germany to western Europe, which we explain with gaseous particle precursors coming with little wet scavenging from this region. Annual emissions for 2009 of PM10, BC, SO2, and NOx were accumulated along each trajectory and compared with the corresponding measured time series. The agreement of each pair of time series was optimized by varying monthly factors and annual factors on the 2009 emissions. This approach yielded broader summer emission minima than published values that were partly displaced from the midsummer positions. The validity of connecting the ambient concentration and emission of particulate pollution was tested by calculating temporal changes in eBC for subsets of back trajectories passing over two separate prominent emission regions, region A to the northwest and B to the southeast of the measuring stations. Consistent with reported emission data the calculated emission decreases over region A are significantly stronger than over region B.

Regional-scale modelling for the assessment of atmospheric particulate matter concentrations at rural background locations in Europe

Abstract. The application of regional-scale air quality models is an important tool in air quality assessment and management. For this reason, the understanding of model abilities and performances is mandatory. The main objective of this research was to investigate the spatial and temporal variability of background particulate matter (PM) concentrations, to evaluate the regional air quality modelling performance in simulating PM concentrations during statically stable conditions and to investigate processes that contribute to regionally increased PM concentrations with a focus on eastern and central Europe. The temporal and spatial variability of observed PM was analysed at 310 rural background stations in Europe during 2011. Two different regional air quality modelling systems (offline coupled European Monitoring and Evaluation Programme, EMEP, and online coupled Weather Research and Forecasting with Chemistry) were applied to simulate the transport of pollutants and to further investigate the processes that contributed to increased concentrations during high-pollution episodes. Background PM measurements from rural background stations, wind speed, surface pressure and ambient temperature data from 920 meteorological stations across Europe, classified according to the elevation, were used for the evaluation of individual model performance. Among the sea-level stations (up to 200 m), the best modelling performance, in terms of meteorology and chemistry, was found for both models. The underestimated modelled PM concentrations in some cases indicated the importance of the accurate assessment of regional air pollution transport under statically stable atmospheric conditions and the necessity of further model improvements.

Observed Relationships Between the Urban Heat Island, Urban Pollution Island, and Downward Longwave Radiation in the Beijing Area

AbstractWe used the mean air temperature and particulate matter concentration at northern and southern rural stations as rural background values to calculate the urban heat island intensity (UHII) and urban pollution island intensity (UPII) for Beijing. The correlation between UHII and UPII is significantly negative in winter during the daytime and nighttime when selecting southern rural background stations but significantly positive in spring during both daytime and nighttime and in winter during the nighttime when selecting northern rural background stations. The downward longwave radiation (DLR) is highly correlated with surface air temperature and water vapor, and with particulate matter concentration in winter and summer. Water vapor also has a high correlation with particulate matter concentration in winter and summer. Winter data were used to investigate the particulate matter contribution to DLR to minimize the effect of humidity. The results indicate that in winter the urban area DLR and net radiation increased more than rural area under polluted conditions compared with clean conditions, which may lead to an increase in UHII. But in other seasons with more moisture, the aerosol effect on DLR is smaller than water vapor. Our results imply that the contribution of air pollutants to DLR had been overestimated in recent studies without removing water vapor effects on the longwave radiation. We suggest that the interaction between the urban heat island and the urban pollution island and related mitigation strategies needs to be carefully studied in the future by considering different climate zone and seasons.

Summertime particulate matter and its composition in Greece

During the summer of 2012 a coordinated field campaign was conducted in multiple locations in Greece in order to characterize the ambient particulate matter (PM) levels, its chemical composition and the contribution of the regional and local sources. PM1, PM2.5 and PM10 samples were collected simultaneously at seven different sites in Greece: an urban and a suburban station in Patras, a suburban station in Thessaloniki, a suburban and an urban background station in Athens, a rural background station at the Navarino Environmental Observatory (NEO) in southwestern Peloponnese and a remote background site at Finokalia in the northeastern part of Crete. The sites were selected to facilitate the estimation of the contribution of the local emission sources and long range transport.Sulfate and organics were the major PM1 components in all sites suggesting that high sulfate levels still remain in parts of Europe. The photochemistry of the Eastern Mediterranean can convert rapidly the emitted sulphur dioxide to sulfate. Our analysis indicated significant sulfate production over the area, with high sulfate levels, especially in the remote site of Finokalia, associated with air masses that had passed over Turkey. There was high regional secondary organic aerosol production dominating organic aerosol levels even in a major city like Athens. High organic aerosol levels were associated with air masses that had crossed the Balkans with a significant biogenic component. The average PM2.5 concentration ranged from 13 to 18 μg m−3 in the different sites. There were unexpected significant gradients in the concentrations of secondary aerosol components in length scales of a few hundred kilometers. The low concentrations of measured PM2.5 nitrate are mostly organic nitrates and supermicrometer nitrate associated with sea-salt and dust. Dust was a significant PM10 constituent in all areas and was quite variable in space showing the importance of the local sources.

Effects of ship emissions on air quality in the Baltic Sea region simulated with three different chemistry transport models

Abstract. The Baltic Sea is a highly frequented shipping area with busy shipping lanes close to densely populated regions. Exhaust emissions from ship traffic into the atmosphere do not only enhance air pollution, they also affect the Baltic Sea environment through acidification and eutrophication of marine waters and surrounding terrestrial ecosystems. As part of the European BONUS project SHEBA (Sustainable Shipping and Environment of the Baltic Sea region), the transport, chemical transformation and fate of atmospheric pollutants in the Baltic Sea region were simulated with three regional chemistry transport model (CTM) systems, CMAQ, EMEP/MSC-W and SILAM, with grid resolutions between 4 and 11 km. The main goal was to quantify the effect that shipping emissions have on the regional air quality in the Baltic Sea region when the same shipping emission dataset but different CTMs are used in their typical set-ups. The performance of these models and the shipping contribution to the results of the individual models were evaluated for sulfur dioxide (SO2), nitrogen dioxide (NO2), ozone (O3) and particulate matter (PM2.5). Model results from the three CTMs for total air pollutant concentrations were compared to observations from rural and urban background stations of the AirBase monitoring network in the coastal areas of the Baltic Sea region. Observed PM2.5 in summer was underestimated strongly by CMAQ and to some extent by EMEP/MSC-W. Observed PM2.5 in winter was underestimated by SILAM. In autumn all models were in better agreement with observed PM2.5. The spatial average of the annual mean O3 in the EMEP/MSC-W simulation was ca. 20 % higher compared to the other two simulations, which is mainly the consequence of using a different set of boundary conditions for the European model domain. There are significant differences in the calculated ship contributions to the levels of air pollutants among the three models. EMEP/MSC-W, with the coarsest grid, predicted weaker ozone depletion through NO emissions in the proximity of the main shipping routes than the other two models. The average contribution of ships to PM2.5 levels in coastal land areas is in the range of 3.1 %–5.7 % for the three CTMs. Differences in ship-related PM2.5 between the models are mainly attributed to differences in the schemes for inorganic aerosol formation. Differences in the ship-related elemental carbon (EC) among the CTMs can be explained by differences in the meteorological conditions, atmospheric transport processes and the applied wet-scavenging parameterizations. Overall, results from the present study show the sensitivity of the ship contribution to combined uncertainties in boundary conditions, meteorological data and aerosol formation and deposition schemes. This is an important step towards a more reliable evaluation of policy options regarding emission regulations for ship traffic and the planned introduction of a nitrogen emission control area (NECA) in the Baltic Sea and the North Sea in 2021.

Seasonal study of stable carbon and nitrogen isotopic composition in fine aerosols at a Central European rural background station

Abstract. A study of the stable carbon isotope ratios (δ13C) of total carbon (TC) and the nitrogen isotope ratios (δ15N) of total nitrogen (TN) was carried out for fine aerosol particles (PM1) and was undertaken every 2 days with a 24 h sampling period at a rural background site in Košetice (Central Europe) from 27 September 2013 to 9 August 2014 (n=146). We found a seasonal pattern for both δ13C and δ15N. The seasonal variation in δ15N was characterized by lower values (average of 13.1±4.5 ‰) in winter and higher values (25.0±1.6 ‰) in summer. Autumn and spring were transition periods when the isotopic composition gradually changed due to the changing sources and ambient temperature. The seasonal variation in δ13C was less pronounced but more depleted in 13C in summer (-27.8±0.4 ‰) as compared to winter (-26.7±0.5 ‰). A comparative analysis with water-soluble ions, organic carbon, elemental carbon, trace gases and meteorological parameters (mainly ambient temperature) has shown major associations with the isotopic compositions, which has provided greater knowledge and understanding of the corresponding processes. A comparison of δ15N with NO3-, NH4+ and organic nitrogen (OrgN) revealed that although a higher content of NO3- was associated with a decrease in the δ15N of TN, NH4+ and OrgN caused increases. The highest concentrations of nitrate, mainly represented by NH4NO3 related to the emissions from biomass burning leading to an average δ15N of TN (13.3 ‰) in winter. During spring, the percentage of NO3- in PM1 decreased. An enrichment of 15N was probably driven by the equilibrium exchange between the gas and aerosol phases (NH3(g) ↔ NH4+(p)), which is supported by the increased ambient temperature. This equilibrium was suppressed in early summer when the molar ratios of NH4+/SO42- reached 2, and the nitrate partitioning in aerosol was negligible due to the increased ambient temperature. Summertime δ15N values were among the highest, suggesting the aging of ammonium sulfate and OrgN aerosols. Such aged aerosols can be coated by organics in which 13C enrichment takes place by the photooxidation process. This result was supported by a positive correlation of δ13C with ambient temperature and ozone, as observed in the summer season. During winter, we observed an event with the lowest δ15N and highest δ13C values. The winter event occurred in prevailing southeast air masses. Although the higher δ13C values probably originated from biomass-burning particles, the lowest δ15N values were probably associated with agriculture emissions of NH3 under low-temperature conditions (< 0 ∘C).

Characteristics, Formation Mechanisms and Potential Transport Pathways of PM2.5 at a Rural Background Site in Chongqing, Southwest China

ABSTRACT Daily PM2.5 samples were collected at a rural background station (JinYun) located in Chongqing across four consecutive seasons from October 2014 to July 2015. The major water-soluble inorganic ions (WSIIs), organic carbon (OC) and elemental carbon (EC) were analyzed, and their chemical characteristics, transport pathways and potential source regions were investigated. The average annual PM2.5 concentration was 56.2 ± 31.0 µg m–3, of which secondary inorganic aerosol (SNA) and carbonaceous aerosols composed 41.0% and 29.4%, respectively. Higher concentrations of and contributions from SO42–, which were likely caused by the secondary transformation of SO2 into SO42–, were observed in summer than in autumn and spring. Additionally, transportation from the urban area of Chongqing (Yubei) played an important role in elevating the SO42– during this season. Although the accumulation of PM2.5 during pollution episodes in winter was also due to aqueous-phase reactions, based on the entire year, NO3– formation may have been primarily driven by homogeneous gas-phase reactions. Furthermore, the aerosol environment was ammonium-rich, and NH4+ formation promoted the production of NO3– at lower temperatures. The carbonaceous component, which consisted of 81.0–84.6% OC, exhibited higher concentrations in winter than in the other seasons; 50.0–77.2% of the total OC, in turn, was contributed by primary organic carbon (POC). Potential source contribution function (PSCF) analysis suggests that the site was mainly affected by regional pollution originating in the southwestern and northern areas of Chongqing.