Urban Background Site Research Articles

Low emission zones reduced PM10 but not NO2 concentrations in Berlin and Munich, Germany

Low emission zones (LEZs) aiming at improving the air quality in urban areas have been implemented in many European cities. However, studies are limited in evaluating the effects of LEZ, and most of which used simple methods. In this study, a general additive mixed model was utilized to account for confounders in the atmosphere and validate the effects of LEZ on PM10 and NO2 concentrations in two German cities. In addition, the effects of LEZ on elemental carbon (EC) and total carbon (TC) in Berlin were also evaluated. The LEZ effects were estimated after taking into account air pollutant concentrations at a reference site located in the regional background, and adjusting for hour of the week, public holidays, season, and wind direction. The LEZ in Berlin, and the LEZ in combination with the heavy-duty vehicle (HDV) transit ban in Munich significantly reduced the PM10 concentrations, at both traffic sites (TS) and urban background sites (UB). The effects were greater in LEZ stage 3 than in LEZ stages 2 and 1. Moreover, compared with PM10, LEZ was more efficient in reducing EC, a component that is considered more toxic than PM10 mass. In contrast, the LEZ had no consistent effect on NO2 levels: no effects were observed in Berlin; in Munich, the combination of the LEZ and the HDV transit ban reduced NO2 at UB site in LEZ stage 1, but without further reductions in subsequent stages of the LEZ. Overall, our study indicated that LEZs, which target the major primary air pollution source in the highly populated city center could be an effective way to improve urban air quality such as PM mass concentration and EC level.

Comparison of PM10 Sources at Traffic and Urban Background Sites Based on Elemental, Chemical and Isotopic Composition: Case Study from Krakow, Southern Poland

In large urban agglomerations, car traffic is one of the main sources of particulate matter. It consists of particulate matter directly generated in the process of incomplete liquid fuel burning in vehicle engine, secondary aerosols formed from exhaust gaseous pollutants (NOx, SO2) as well as products of tires, brake pads and pavement abrasion. Krakow is one of the cities in Europe with the highest concentrations of particulate matter. The article presents the results of combined elemental, chemical and isotopic analyses of particulate matter PM10 at two contrasting urban environments during winter and summer seasons. Daily PM10 samples were collected during the summer and winter seasons of 2018/2019 at two stations belonging to the network monitoring air quality in the city. Mean PM10 concentrations at traffic-dominated stations were equal to 35 ± 7 µg/m3 and 76 ± 28 µg/m3 in summer and winter, respectively, to be compared with 25.6 ± 5.7 µg/m3 and 51 ± 25 µg/m3 in summer and winter, respectively, recorded at the urban background station. The source attribution of analyzed PM10 samples was carried out using two modeling approaches: (i) The Positive Matrix Factorization (PMF) method for elemental and chemical composition (concentrations of elements, ions, as well as organic and elemental carbon in daily PM10 samples), and (ii) Isotope Mass Balance (IMB) for 13C and 14C carbon isotope composition of carbonaceous fraction of PM10. For PMF application, five sources of particulate matter were identified for each station: fossil fuel combustion, secondary inorganic aerosols, traffic exhaust, soil, and the fifth source which included road dust, industry, construction work. The IMB method allowed the partitioning of the total carbon reservoir of PM10 into carbon originating from coal combustion, from biogenic sources (natural emissions and biomass burning) and from traffic. Both apportionment methods were applied together for the first time in the Krakow agglomeration and they gave consistent results.

Insights into Elemental Composition and Sources of Fine and Coarse Particulate Matter in Dense Traffic Areas in Toronto and Vancouver, Canada.

Traffic is a significant pollution source in cities and has caused various health and environmental concerns worldwide. Therefore, an improved understanding of traffic impacts on particle concentrations and their components could help mitigate air pollution. In this study, the characteristics and sources of trace elements in PM2.5 (fine), and PM10-2.5 (coarse), were investigated in dense traffic areas in Toronto and Vancouver, Canada, from 2015–2017. At nearby urban background sites, 24-h integrated PM samples were also concurrently collected. The PM2.5 and PM10-2.5 masses, and a number of elements (i.e., Fe, Ba, Cu, Sb, Zn, Cr), showed clear increases at each near-road site, related to the traffic emissions resulting from resuspension and/or abrasion sources. The trace elements showed a clear partitioning trend between PM2.5 and PM10-2.5, thus reflecting the origin of some of these elements. The application of positive matrix factorization (PMF) to the combined fine and coarse metal data (86 total), with 24 observations at each site, was used to determine the contribution of different sources to the total metal concentrations in fine and coarse PM. Four major sources were identified by the PMF model, including two traffic non-exhaust (crustal/road dust, brake/tire wear) sources, along with regional and local industrial sources. Source apportionment indicated that the resuspended crustal/road dust factor was the dominant contributor to the total coarse-bound trace element (i.e., Fe, Ti, Ba, Cu, Zn, Sb, Cr) concentrations produced by vehicular exhaust and non-exhaust traffic-related processes that have been deposited onto the surface. The second non-exhaust factor related to brake/tire wear abrasion accounted for a considerable portion of the fine and coarse elemental (i.e., Ba, Fe, Cu, Zn, Sb) mass at both near-road sites. Regional and local industry contributed mostly to the fine elemental (i.e., S, As, Se, Cd, Pb) concentrations. Overall, the results show that non-exhaust traffic-related processes were major contributors to the various redox-active metal species (i.e., Fe, Cu) in both PM fractions. In addition, a substantial proportion of these metals in PM2.5 was water-soluble, which is an important contributor to the formation of reactive oxygen species and, thus, may lead to oxidative damage to cells in the human body. It appears that controlling traffic non-exhaust-related metals emissions, in the absence of significant point sources in the area, could have a pronounced effect on the redox activity of PM, with broad implications for the protection of public health.

Measurement report: Receptor modeling for source identification of urban fine and coarse particulate matter using hourly elemental composition

Abstract. The elemental composition of the fine (PM2.5) and coarse (PM2.5−10) fraction of atmospheric particulate matter was measured at an hourly time resolution by the use of a streaker sampler during a winter period at a Central European urban background site in Warsaw, Poland. A combination of multivariate (Positive Matrix Factorization) and wind- (Conditional Probability Function) and trajectory-based (Cluster Analysis) receptor models was applied for source apportionment. It allowed for the identification of five similar sources in both fractions, including sulfates, soil dust, road salt, and traffic- and industry-related sources. Another two sources, i.e., Cl-rich and wood and coal combustion, were solely identified in the fine fraction. In the fine fraction, aged sulfate aerosol related to emissions from domestic solid fuel combustion in the outskirts of the city was the largest contributing source to fine elemental mass (44 %), while traffic-related sources, including soil dust mixed with road dust, road dust, and traffic emissions, had the biggest contribution to the coarse elemental mass (together accounting for 83 %). Regional transport of aged aerosols and more local impact of the rest of the identified sources played a crucial role in aerosol formation over the city. In addition, two intensive Saharan dust outbreaks were registered on 18 February and 8 March 2016. Both episodes were characterized by the long-range transport of dust at 1500 and 3000 m over Warsaw and the concentrations of the soil component being 7 (up to 3.5 µg m−3) and 6 (up to 6.1 µg m−3) times higher than the mean concentrations observed during non-episodes days (0.5 and 1.1 µg m−3) in the fine and coarse fractions, respectively. The set of receptor models applied to the high time resolution data allowed us to follow, in detail, the daily evolution of the aerosol elemental composition and to identify distinct sources contributing to the concentrations of the different PM fractions, and it revealed the multi-faceted nature of some elements with diverse origins in the fine and coarse fractions. The hourly resolution of meteorological conditions and air mass back trajectories allowed us to follow the transport pathways of the aerosol as well.

Personal exposure levels to O3, NOx and PM10 and the association to ambient levels in two Swedish cities

Exposure to air pollution is of great concern for public health although studies on the associations between exposure estimates and personal exposure are limited and somewhat inconsistent. The aim of this study was to quantify the associations between personal nitrogen oxides (NOx), ozone (O3) and particulate matter (PM10) exposure levels and ambient levels, and the impact of climate and time spent outdoors in two cities in Sweden. Subjects (n = 65) from two Swedish cities participated in the study. The study protocol included personal exposure measurements at three occasions, or waves. Personal exposure measurements were performed for NOx and O3 for 24 h and PM10 for 24 h, and the participants kept an activity diary. Stationary monitoring stations provided hourly data of NOx, O3 and PM, as well as data on air temperature and relative humidity. Data were analysed using mixed linear models with the subject-id as a random effect and stationary exposure and covariates as fixed effects. Personal exposure levels of NOx, O3 and PM10 were significantly associated with levels measured at air pollution monitoring stations. The associations persisted after adjusting for temperature, relative humidity, city and wave, but the modelled estimates were slightly attenuated from 2.4% (95% CI 1.8–2.9) to 2.0% (0.97–2.94%) for NOx, from 3.7% (95% CI 3.1–4.4) to 2.1% (95% CI 1.1–2.9%) for O3 and from 2.6% (95% 0.9–4.2%) to 1.3% (95% CI − 1.5–4.0) for PM10. After adding covariates, the degree of explanation offered by the model (coefficient of determination, or R2) did not change for NOx (0.64 to 0.63) but increased from 0.46 to 0.63 for O3, and from 0.38 to 0.43 for PM10. Personal exposure to NOx, O3 and PM has moderate to good association with levels measured at urban background sites. The results indicate that stationary measurements are valid as measure of exposure in environmental health risk assessments, especially if they can be refined using activity diaries and meteorological data. Approximately 50–70% of the variation of the personal exposure was explained by the stationary measurement, implying occurrence of misclassification in studies using more crude exposure metrics, potentially leading to underestimates of the effects of exposure to ambient air pollution.

Effect of aerosol types from various sources at an urban location on spectral curvature of scattering and absorption coefficients

This study analyzes the spectral characteristics of in situ measured aerosol properties, namely scattering, absorption and single scattering albedo (SSA), explicitly examining the curvature characteristics of their wavelength dependence. Measurements were performed at an urban background site in Athens, Greece, during December 2017 and March 2018 characterized by contrasting aerosol sources and types, i.e. residential wood burning (RWB) and desert dust, respectively, which modulate the urban conditions, that are typically dominated by fossil-fuel combustion. Aerosol types were classified via the Scattering Ångström Exponent (SAE) vs. Absorption Ångström Exponent (AAE) matrix, with the black carbon (BC)-dominated type displaying the highest fraction (~40%) in both periods. The spectral optical properties were examined for each aerosol type and month, revealing notable differences, which are closely linked to the contrasting emission sources, atmospheric dynamics and mixing processes. BC from fossil-fuel emissions and regional background aerosols mostly presented similar characteristics in both months. Emphasis was given on the spectral curvature effect, since the different aerosol types display notable changes in the spectral dependence of scattering and absorption in logarithmic coordinates. The enhanced presence of brown carbon resulted in negative curvature for scattering (concave curves) and highly positive for absorption (convex curves), while the presence of BC was mostly translated in a better fit of the Ångström formula and small curvature effects. Intense dust events resulted in positive curvature for absorption and mostly negative for scattering. A scatterplot between the wavelength dependence of SSA and the scattering curvature may further differentiate key aerosol types i.e. BC, brown carbon and dust. This study highlights the curvature effects of the scattering, absorption and SSA, which have not been adequately addressed yet. The approach provides new insights in the differentiation of source-related aerosol types, although more analysis is needed to examine if findings are reproduced in other environments.

How to obtain large amounts of location- and time-specific PM2.5 with homogeneous mass and composition? A possible approach, from particulate collection to chemical characterization

A suitable protocol for the collection, extraction, and characterization of a large quantity of a local and current fine particulate matter (PM2.5) was developed, to provide homogeneous PM2.5 amounts for use in in vitro and in vivo toxicological assays rather than a generic and obsolete standard reference material (SRM). PM2.5 samples were collected at an outdoor urban background site in Como, Northern Italy, using a high-volume air sampler (500 L/min) equipped with polytetrafluoroethylene (PTFE)-coated glass fiber filters (eight sampling campaigns of 24–96 h each, from February to April 2019). PM2.5 was extracted from the filters by sequential sonication steps and the final pooled extract was filtered to remove the glass fibers released during extraction. Several PM2.5 aliquots (n = 55) were then prepared from the PM2.5 dry residue for i) a chemical characterization of the elements, inorganic ions, and the carbonaceous fraction and ii) in vivo and in vitro studies. The proposed protocol allowed a large amount of ambient PM2.5 (>300 mg) to be collected within a reasonably short time. An average extraction efficiency of 75% was achieved, and the chemical analyses conducted on a set of PM2.5-replicates revealed a satisfactory level of precision, ranging from 3% (anions and OC) to 10% (trace metals and EC), thereby confirming the possibility of obtaining aliquots with homogeneous mass and composition. Finally, the emerging differences with the SRM 1648a elemental composition suggest the importance of location- and time-specific particulate testing, which is truly representative of the actual exposure scenario for specific populations.

Source-specific light absorption by carbonaceous components in the complex aerosol matrix from yearly filter-based measurements

Abstract. Understanding the sources of light-absorbing organic (brown) carbon (BrC) and its interaction with black carbon (BC) and other non-refractory particulate matter (NR-PM) fractions is important for reducing uncertainties in the aerosol direct radiative forcing. In this study, we combine multiple filter-based techniques to achieve long-term, spectrally resolved, source- and species-specific atmospheric absorption closure. We determine the mass absorption efficiency (MAE) in dilute bulk solutions at 370 nm to be equal to 1.4 m2 g−1 for fresh biomass smoke, 0.7 m2 g−1 for winter-oxygenated organic aerosol (OA), and 0.13 m2 g−1 for other less absorbing OA. We apply Mie calculations to estimate the contributions of these fractions to total aerosol absorption. While enhanced absorption in the near-UV has been traditionally attributed to primary biomass smoke, here we show that anthropogenic oxygenated OA may be equally important for BrC absorption during winter, especially at an urban background site. We demonstrate that insoluble tar balls are negligible in residential biomass burning atmospheric samples of this study and thus could attribute the totality of the NR-PM absorption at shorter wavelengths to methanol-extractable BrC. As for BC, we show that the mass absorption cross-section (MAC) of this fraction is independent of its source, while we observe evidence for a filter-based lensing effect associated with the presence of NR-PM components. We find that bare BC has a MAC of 6.3 m2 g−1 at 660 nm and an absorption Ångström exponent of 0.93 ± 0.16, while in the presence of coatings its absorption is enhanced by a factor of ∼ 1.4. Based on Mie calculations of closure between observed and predicted total light absorption, we provide an indication for a suppression of the filter-based lensing effect by BrC. The total absorption reduction remains modest, ∼ 10 %–20 % at 370 nm, and is restricted to shorter wavelengths, where BrC absorption is significant. Overall, our results allow an assessment of the relative importance of the different aerosol fractions to the total absorption for aerosols from a wide range of sources and atmospheric ages. When integrated with the solar spectrum at 300–900 nm, bare BC is found to contribute around two-thirds of the solar radiation absorption by total carbonaceous aerosols, amplified by the filter-based lensing effect (with an interquartile range, IQR, of 8 %–27 %), while the IQR of the contributions by particulate BrC is 6 %–13 % (13 %–20 % at the rural site during winter). Future studies that will directly benefit from these results include (a) optical modelling aiming at understanding the absorption profiles of a complex aerosol composed of BrC, BC and lensing-inducing coatings; (b) source apportionment aiming at understanding the sources of BC and BrC from the aerosol absorption profiles; (c) global modelling aiming at quantifying the most important aerosol absorbers.

Morphological properties, chemical composition, cancer risks and toxicological potential of airborne particles from traffic and urban background sites

From a sampling campaign from December 2018 to June 2019, at a traffic and an urban background site in Coimbra, Portugal, two particulate matter (PM10) samples from each month were selected to characterise the morphology by scanning electron microscopy, to determine the organic and inorganic chemical composition by multiple analytical techniques and to assess the ecotoxicity by the Vibrio fischeri bioluminescence inhibition assay. PM10 concentrations in winter were approximately twice as high as those recorded in the spring. Biomass burning was the greatest contributor to air pollution in winter at both sites. The contribution of vehicle emissions to the PM10 at the roadside was, on average, 7 times higher than at the background location. Distinct particle morphologies were observed. Higher abundances of aggregates enriched in Fe, Ti, Ba, Cr, Co, Cu, Zr, Mn and soot particles were registered in samples from the roadside. Bivariate plots suggested common sources of PAHs, mostly traffic and biomass burning, across the city. Benzo[a]pyrene equivalent concentrations were within the values documented for other European cities. Cancer risks resulting from exposure to PAHs by inhalation were estimated to be low (10−6 ≤ to <10−4) for both sites. The noncarcinogenic risks from particulate trace elements were always higher than the target value of 1. Cancer risks for Cr were found to be higher than the acceptable level (10−6). The calculation of toxic units indicated that 64% of the samples from the roadside location were toxic and 14% very toxic, while the corresponding shares for the urban background site were 50% and 7%, respectively. Many PM10-bound constituents, especially markers of biomass burning (e.g. anhydrosugars) and traffic emissions (e.g. Fe, Cu, Zn), showed significant statistical correlations with toxicity.

Sources of airborne particulates (PM10) in the port city of Rijeka, Croatia.

The air quality monitoring in Rijeka started in the early 1970s and has been oriented to air pollution caused by the big industrial sources (new petroleum refinery, oil burning power plant, coke plant), while maritime traffic was neglected. First emission inventory comprising port emission was done only in 2008 indicating similar level of emissions as road traffic. Further analyses on maritime impact were done within MED project POSEIDON. This was the good opportunity to perform positive matrix factorization (PMF) analysis on airborne particulate data and identify principal sources of pollution within the Rijeka urban area. PMF analyses of PM10 collected from the urban background site in the period 2008-2010 identified 5 factors: biomass burning, secondary sulphates, sea spray, road/soil dust and metal industry/traffic. Condition probability functions (CPF) obtained from PMF factors of dust and secondary sulphates indicate that Ca, Fe, Zn and Cu originate from harbour area due to reloading of fertilizers and metal waste, as well as SO42- and NH4+ pointing to maritime corridor leading to the Rijeka harbour. These data could not quantify the maritime impact on the air quality, but gave the first estimation of contribution of various sources to air pollution within the Rijeka Bay area. The maritime contribution to air quality was estimated in other part of the same project, as primary PM2.5 emission obtained from vanadium. Both primary PM2.5 emission and polynuclear aromatic hydrocarbon profiles indicated reduced economic activity, including maritime traffic, during economic crisis in the period 2008-2012.

Automated identification and quantification of tire wear particles (TWP) in airborne dust: SEM/EDX single particle analysis coupled to a machine learning classifier

The share of non-exhaust particles, including tire wear particles (TWP), within the airborne dust and particularly within PM10 has increased in recent years due to a significant reduction of other particles including exhaust road traffic emissions. However, the quantification of TWP is a demanding task due to the non-specificity of tracers, and the fact that they are commonly contained in analytically challenging low concentrations (e.g. Zn, styrene, 1,3-butadiene, vinylcyclohexene). This difficulty is amplified by the chemical and morpho-textural heterogeneity of TWP resulting from the interaction between the tires and the road surface. In contrast to bulk techniques, automated single particle SEM/EDX analysis can benefit from the ubiquitous heterogeneity of environmental TWP as a diagnostic criterion for their identification and quantification. For this purpose, we follow a machine-learning (ML) approach that makes use of an extensive number (67) of morphological, textural (backscatter-signal based) and chemical descriptors to differentiate environmental particles into the following classes: TWP, metals, minerals and biogenic/organic. We present a ML-based model developed to classify airborne samples (trained by >100,000 environmental particles including 6841 TWP), and its application within a one-year monitoring campaign at two Swiss sites. In this study, the mass concentrations of TWP in the airborne fractions PM80-10, PM10-2.5 and PM2.5-1 were determined. Furthermore, the particle size distribution and shape characteristics of 5621 TWP were evaluated. A cut through a TWP by means of FIB-SEM evidences that the mineral and metal particles typically found in TWP are not only present on the particle surface but also throughout the complete TWP volume. At the urban background site, the annual average mass fraction of TWP and micro-rubber in PM10 was 1.8% (0.28 μg/m3) and 0.9%, respectively. At the urban kerbside site, the corresponding values were 6 times higher amounting to 10.5% (2.24 μg/m3) for TWP, and 5.0% for micro-rubber.

A phenomenology of new particle formation (NPF) at 13 European sites

Abstract. New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially, and this variability is yet to be fully understood. In the present study, long-term particle size distribution datasets (minimum of 3 years) from 13 sites of various land uses and climates from across Europe were studied, and NPF events, deriving from secondary formation and not traffic-related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides (though in many cases differences between the sites were small), underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found, even at sites in close proximity (&lt; 200 km), due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400 % at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity, or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions.

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.

NPAHs and OPAHs in the atmosphere of two central European cities: Seasonality, urban-to-background gradients, cancer risks and gas-to-particle partitioning

Derivatives of polycyclic aromatic hydrocarbons (PAHs) such as nitrated- and oxygenated-PAHs (NPAHs and OPAHs) could be even more toxic and harmful for the environment and humans than PAHs. We assessed the spatial and seasonal variations of NPAHs and OPAHs atmospheric levels, their cancer risks and their gas-to-particle partitioning. To this end, about 250 samples of fine particulate matter (PM2.5) and 50 gaseous samples were collected in 2017 in central Europe in the cities of Brno and Ljubljana (two traffic and two urban background sites) as well as one rural site.The average particulate concentrations were ranging from below limit of quantification to 593 pg m−3 for Σ9NPAHs and from 1.64 to 4330 pg m−3 for Σ11OPAHs, with significantly higher concentrations in winter compared to summer.In winter, the particulate levels of NPAHs and OPAHs were higher at the traffic site compared to the urban background site in Brno while the opposite was found in Ljubljana. NPAHs and OPAHs particulate levels were influenced by the meteorological parameters and co-varied with several air pollutants. The significance of secondary formation on the occurrence of some NPAHs and OPAHs is indicated. In winter, 27–47% of samples collected at all sites were above the acceptable lifetime carcinogenic risk. The gas-particle partitioning of NPAHs and OPAHs was influenced by their physico-chemical properties, the season and the site-specific aerosol composition. Three NPAHs and five OPAHs had higher particulate mass fractions at the traffic site, suggesting they could be primarily emitted as particles from vehicle traffic and subsequently partitioning to the gas phase along air transport. This study underlines the importance of inclusion of the gas phase in addition to the particulate phase when assessing the atmospheric fate of polycyclic aromatic compounds and also when assessing the related health risk.

Urban aerosol size distributions: a global perspective

Abstract. Urban aerosol measurements are necessary to establish associations between air pollution and human health outcomes and to evaluate the efficacy of air quality legislation and emissions standards. The measurement of urban aerosol particle size distributions (PSDs) is of particular importance as they enable characterization of size-dependent processes that govern a particle's transport, transformation, and fate in the urban atmosphere. PSDs also improve our ability to link air pollution to health effects through evaluation of particle deposition in the respiratory system and inhalation toxicity. To inform future measurements of urban aerosol observations, this paper reviews and critically analyzes the current state of knowledge on urban aerosol PSD measurements by synthesizing 737 PSD observations made between 1998 to 2017 in 114 cities in 43 countries around the globe. Significant variations in the shape and magnitude of urban aerosol number and mass PSDs were identified among different geographical regions. In general, number PSDs in Europe (EU) and North America, Australia, and New Zealand (NAAN) are dominated by nucleation- and Aitken-mode particles. PSDs in Central, South, and Southeast Asia (CSSA) and East Asia (EA) are shifted to larger sizes, with a meaningful contribution from the accumulation mode. Urban mass PSDs are typically bimodal, presenting a dominant mode in the accumulation mode and a secondary mode in the coarse mode. Most PSD observations published in the literature are short-term, with only 14 % providing data for longer than 6 months. There is a paucity of PSDs measured in Africa (AF), CSSA, Latin America (LA), and West Asia (WA), demonstrating the need for long-term aerosol measurements across wide size ranges in many cities around the globe. Geographical variations in urban aerosol effective densities were also reviewed. Size-resolved urban aerosol effective density functions from 3 to 10 000 nm were established for different geographical regions and intra-city sampling locations in order to accurately translate number PSDs to mass PSDs, with significant variations observed between near-road and urban background sites. The results of this study demonstrate that global initiatives are urgently needed to develop infrastructure for routine and long-term monitoring of urban aerosol PSDs spanning the nucleation to coarse mode. Doing so will advance our understanding of spatiotemporal trends in urban PSDs throughout the world and provide a foundation to more reliably elucidate the impact of urban aerosols on atmospheric processes, human health, and climate.

Assessing the sources of particles at an urban background site using both regulatory instruments and low-cost sensors – a comparative study

Abstract. Measurement and source apportionment of atmospheric pollutants are crucial for the assessment of air quality and the implementation of policies for their improvement. In most cases, such measurements use expensive regulatory-grade instruments, which makes it difficult to achieve wide spatial coverage. Low-cost sensors may provide a more affordable alternative, but their capability and reliability in separating distinct sources of particles have not been tested extensively yet. The present study examines the ability of a low-cost optical particle counter (OPC) to identify the sources of particles and conditions that affect particle concentrations at an urban background site in Birmingham, UK. To help evaluate the results, the same analysis is performed on data from a regulatory-grade instrument (SMPS, scanning mobility particle sizer) and compared to the outcomes from the OPC analysis. The analysis of the low-cost sensor data manages to separate periods and atmospheric conditions according to the level of pollution at the site. It also successfully identifies a number of sources for the observed particles, which were also identified using the regulatory-grade instruments. The low-cost sensor, due to the particle size range measured (0.35 to 40 µm), performed rather well in differentiating sources of particles with sizes greater than 1 µm, though its ability to distinguish their diurnal variation, as well as to separate sources of smaller particles, at the site was limited. The current level of source identification demonstrated makes the technique useful for background site studies, where larger particles with smaller temporal variations are of significant importance. This study highlights the current capability of low-cost sensors in source identification and differentiation using clustering approaches. Future directions towards particulate matter source apportionment using low-cost OPCs are highlighted.

Consistent determination of the heating rate of light-absorbing aerosol using wavelength- and time-dependent Aethalometer multiple-scattering correction

Accurate and temporally consistent measurements of light absorbing aerosol (LAA) heating rate (HR) and of its source apportionment (fossil-fuel, FF; biomass-burning, BB) and speciation (black and brown Carbon; BC, BrC) are needed to evaluate LAA short-term climate forcing. For this purpose, wavelength- and time-dependent accurate LAA absorption coefficients are required. HR was experimentally determined and apportioned (sources/species) in the EMEP/ACTRIS/COLOSSAL-2018 winter campaign in Milan (urban-background site). Two Aethalometers (AE31/AE33) were installed together with a MAAP, CPC, OPC, a low volume sampler (PM2.5) and radiation instruments. AE31/AE33 multiple-scattering correction factors (C) were determined using two reference systems for the absorption coefficient: 1) 5-wavelength PP_UniMI with low time resolution (12 h, applied to PM2.5 samples); 2) timely-resolved MAAP data at a single wavelength. Using wavelength- and time-independent C values for the AE31 and AE33 obtained with the same reference device, the total HR showed a consistency (i.e. reproducibility) with average values comparable at 95% probability. However, if different reference devices/approaches are used, i.e. MAAP is chosen as reference instead of a PP_UniMI, the HR can be overestimated by 23–30% factor (by both AE31/AE33). This became more evident focusing on HR apportionment: AE33 data (corrected by a wavelength- and time-independent C) showed higher HRFF (+24 ± 1%) and higher HRBC (+10 ± 1%) than that of AE31. Conversely, HRBB and HRBrC were −28 ± 1% and −29 ± 1% lower for AE33 compared to AE31. These inconsistencies were overcome by introducing a wavelength-dependent Cλ for both AE31 and AE33, or using multi-wavelength apportionment methods, highlighting the need for further studies on the influence of wavelength corrections for HR determination.Finally, the temporally-resolved determination of C resulted in a diurnal cycle of the HR not statistically different whatever the source- speciation- apportionment used.

Water-insoluble carbonaceous components in rainwater over an urban background location in Northern India during pre-monsoon and monsoon seasons.

The carbonaceous content of rainwater was investigated in samples collected at an urban background site in northern India. Sampling was performed on an event basis during two seasons: pre-monsoon (PM) and monsoon (MN) season covering May-June and July-August, respectively, in 2016. The concentrations of different fractions of water-insoluble organic carbon (WIOC) and elemental carbon (EC) were precisely determined, and the sources of WIOC and EC were also analysed. The result revealed that the average WIOC and EC concentration in rainwater ranged from 0.4 to 52 mgC/L and from 0.1 to 15.3 mgC/L, respectively. The concentrations of WIOC and EC were found to be ~ 9 times and ~ 12 times higher, respectively, in the PM season than MN season. The WIOC/EC ratio indicated higher variation in PM season as compared to that of the MN season, suggesting divergent emission sources during the PM season. The formation of water-insoluble secondary organic carbon (WISOC) has also been identified as one of the causes for the extensive difference in the WIOC/EC ratio in different seasons. Results showed that the WIOC and its fractions were efficiently scavenged through rain. While EC and its fractions were less significantly scavenged, due to its hydrophobicity and fine size. The atmospheric scavenging coefficients of selected carbonaceous components were found significantly correlated with rain intensity (RI) during both the seasons. Higher rain intensity caused greater rates of carbonaceous component wash-out and decreasing concentrations of carbonaceous components in the rain.

Impacts of the COVID-19 lockdown on air pollution at regional and urban background sites in northern Italy

Abstract. The COVID-19 lockdown measures gradually implemented in Lombardy (northern Italy) from 23 February 2020 led to a downturn in several economic sectors with possible impacts on air quality. Several communications claimed in the first weeks of March 2020 that the mitigation in air pollution observed at that time was actually related to these lockdown measures without considering that seasonal variations in emissions and meteorology also influence air quality. To determine the specific impact of lockdown measures on air quality in northern Italy, we compared observations from the European Commission Atmospheric Observatory of Ispra (regional background) and from the regional environmental protection agency (ARPA) air monitoring stations in the Milan conurbation (urban background) with expected values for these observations using two different approaches. On the one hand, intensive aerosol variables determined from specific aerosol characterisation observations performed in Ispra were compared to their 3-year averages. On the other hand, ground-level measured concentrations of atmospheric pollutants (NO2, PM10, O3, NO, SO2) were compared to expected concentrations derived from the Copernicus Atmosphere Monitoring Service Regional (CAMS) ensemble model forecasts, which did not account for lockdown measures. From these comparisons, we show that NO2 concentrations decreased as a consequence of the lockdown by −30 % and −40 % on average at the urban and regional background sites, respectively. Unlike NO2, PM10 concentrations were not significantly affected by lockdown measures. This could be due to any decreases in PM10 (and PM10 precursors) emissions from traffic being compensated for by increases in emissions from domestic heating and/or from changes in the secondary aerosol formation regime resulting from the lockdown measures. The implementation of the lockdown measures also led to an increase in the highest O3 concentrations at both the urban and regional background sites resulting from reduced titration of O3 by NO. The relaxation of the lockdown measures beginning in May resulted in close-to-expected NO2 concentrations in the urban background and to significant increases in PM10 in comparison to expected concentrations at both regional and urban background sites.

Characterization of PM10-Bound Polycyclic Aromatic Hydrocarbons and Associated Carcinogenic Risk in Bangkok, Thailand

Concentrations of ambient particulate-bound polycyclic aromatic hydrocarbons (pPAHs) were measured in PM10 samples collected at roadside, industrial and urban background sites in Bangkok between May 2013 and May 2014. The annual average PM10 concentrations were not significantly different between the roadside (56.4 ± 27.3 µg m−3) and industrial (51.0 ± 31.1 µg m−3) sites. The lowest annual mean PM10 was observed at the urban background site (39.8 ± 22.2 µg m−3). Seasonal variations of pPAHs were observed at the three sampling sites. The total pPAHs ranged between 1.09 and 13.10 ng m−3 (mean 4.85 ± 2.51 ng m−3), 1.49 and 9.39 ng m−3 (mean 3.84 ± 2.01 ng m−3) and 0.77 and 5.20 ng m−3 (mean 2.28 ± 1.16 ng m−3) at the roadside, industrial and urban background sites, respectively. The observed annual average benzo[a]pyrene concentrations were 0.47 ± 0.39 ng m−3, 0.35 ± 0.27 ng m−3 and 0.24 ± 0.19 ng m−3 at the roadside, industrial and urban background sites. Long-term carcinogenic health risk of inhalation exposure expressed as the toxicity equivalent to benzo[a]pyrene concentrations were calculated as 0.83, 0.72 and 0.39 ng m−3 at the industrial, roadside and urban background sites, respectively. The composition of pPAHs plays an important role in the carcinogenicity of a PAHs mixture.