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The evolution of fine aerosol (PM1) species as well as the contribution of potential sources to the total organic aerosol (OA) at an urban background site in Barcelona, in the western Mediterranean basin (WMB) was investigated. For this purpose, a quadrupole aerosol chemical speciation monitor (Q-ACSM) was deployed to acquire real-time measurements for two 1-year periods: May 2014–May 2015 (period A) and September 2017–October 2018 (period B). Total PM1 concentrations showed a slight decrease (from 10.1 to 9.6 µg m−3 from A to B), although the relative contribution of inorganic and organic compounds varied significantly. Regarding inorganic compounds, SO2−4, black carbon (BC) and NH+4 showed a significant decrease from period A to B (−21 %, −18 % and −9 %, respectively), whilst NO−3 concentrations were higher in B (+8 %). Source apportionment revealed OA contained 46 % and 70 % secondary OA (SOA) in periods A and B, respectively. Two secondary oxygenated OA sources (OOA) were differentiated by their oxidation status (i.e. ageing): less oxidized (LO-OOA) and more oxidized (MO-OOA). Disregarding winter periods, when LO-OOA production was not favoured, LO-OOA transformation into MO-OOA was found to be more effective in period B. The lowest LO-OOA-to-MO-OOA ratio, excluding winter, was in September–October 2018 (0.65), implying an accumulation of aged OA after the high temperature and solar radiation conditions in the summer season. In addition to temperature, SOA (sum of OOA factors) was enhanced by exposure to NOx-polluted ambient and other pollutants, especially to O3 and during afternoon hours. The anthropogenic primary OA sources identified, cooking-related OA (COA), hydrocarbon-like OA (HOA), and biomass burning OA (BBOA), decreased from period A to B in both absolute concentrations and relative contribution (as a whole, 44 % and 30 %, respectively). However, their concentrations and proportion to OA grew rapidly during highly polluted episodes. The influence of certain atmospheric episodes on OA sources was also assessed. Both SOA factors were boosted with long- and medium-range circulations, especially those coming from inland Europe and the Mediterranean (triggering mainly MO-OOA) and summer breeze-driven regional circulation (mainly LO-OOA). In contrast, POA was enhanced either during air-renewal episodes or stagnation anticyclonic events. ; Acknowledgements Jordi Massagué is acknowledged for providing the O3 data from the Autonomous Government of Catalonia. IDAEA-CSIC is a Centre of Excellence Severo Ochoa (Spanish Ministry of Science and Innovation, Project CEX2018-000794-S). Financial support This work was supported by COST Action CA16109 COLOSSAL, the Generalitat de Catalunya (grant no. AGAUR 2017 SGR41), the Spanish Ministry of Science and Innovation 70 through the CAIAC project (grant no. PID2019-108990RB-I00), and FEDER funds through EQC2018-004598-P. ; Peer reviewed

In this work for the first time data from two twin stations (Barcelona, urban background, and Montseny, regional background), located in NE of Spain, were used to study the trends of the concentrations of different chemical species in PM10 and PM2.5 along with the trends of the PM10 source contributions from Positive Matrix Factorization (PMF) model. Eleven years of chemical data (2004–2014) were used for this study. Trends of both specie concentrations and source contributions were studied using the Mann-Kendall test for linear trends and a new approach based on multi-exponential fit of the data. Despite the fact that different PM fractions (PM1, PM2.5, PM10) showed linear decreasing trends at both stations, the contributions of specific sources of pollutants and the related chemical tracers showed exponential (single or double) decreasing trends. The different types of trends observed reflected the different effectiveness and/or time of implementation of the measures taken to reduce the concentrations of atmospheric pollutants (i.e. those implemented in the Industrial Emission Directives and in the Large Combustion Plants Directive). Moreover, the trends of the contributions from specific sources such as those related with industrial activities and with primary energy consumption mirrored the effect of the financial crisis in Spain from 2008. The sources that showed statistically significant downward trends at both Barcelona (BCN) and Montseny (MSY) during 2004–2014 were Ammonium sulfate, Ammonium nitrate, and V-Ni bearing source. The contributions from these sources decreased exponentially during the considered period indicating that the observed decrease was not gradual and consistent over time. Moreover, statistically significant decreasing trends were observed for the contributions to PM from the Industrial/Traffic source at MSY (mixed metallurgy and road traffic) and from the Industrial (metallurgy mainly) source at BCN. These sources were clearly linked with anthropogenic activities and the observed decreasing trends confirmed the effectiveness of pollution control measures implemented at EU or regional/local levels. The general trends observed for the calculated PMF source contributions well reflected the trends observed for the chemical tracers of these pollutant sources. ; This work was supported by the MINECO (Spanish Ministry of Economy and Competitiveness), the MAGRAMA (Spanish Ministry of Agriculture, Food and Environment), the Generalitat de Catalunya (AGAUR 2014 SGR33 and the DGQA) and FEDER funds under the PRISMA project (CGL2012‐39623‐ C02/00). The research leading to these results has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement No 654109 and previously from the European Union Seventh Framework Programme (FP7/2007‐2013) under grant agreement n° 262254. NO2 map analyses and visualizations used in this paper were produced with the Giovanni online data system, developed and maintained by the NASA GES DISC. The authors would like to express their gratitude to D. C. Carslaw and K. Ropkins for providing the Openair software used in this paper (Carslaw and Ropkins, 2012; Carslaw, 2012). ; Peer reviewed

Lockdown measures came into force in Spain from March 14th, two weeks after the start of the SARS-CoV-2 epidemic, to reduce the epidemic curve. Our study aims to describe changes in air pollution levels during the lockdown measures in the city of Barcelona (NE Spain), by studying the time evolution of atmospheric pollutants recorded at the urban background and traffic air quality monitoring stations. After two weeks of lockdown, urban air pollution markedly decreased but with substantial differences among pollutants. The most significant reduction was estimated for BC and NO2 (−45 to −51%), pollutants mainly related to traffic emissions. A lower reduction was observed for PM10 (−28 to −31.0%). By contrast, O3 levels increased (+33 to +57% of the 8 h daily maxima), probably due to lower titration of O3 by NO and the decrease of NOx in a VOC-limited environment. Relevant differences in the meteorology of these two periods were also evidenced. The low reduction for PM10 is probably related to a significant regional contribution and the prevailing secondary origin of fine aerosols, but an in-depth evaluation has to be carried out to interpret this lower decrease. There is no defined trend for the low SO2 levels, probably due to the preferential reduction in emissions from the least polluting ships. A reduction of most pollutants to minimal concentrations are expected for the forthcoming weeks because of the more restrictive actions implemented for a total lockdown, which entered into force on March 30th. There are still open questions on why PM10 levels were much less reduced than BC and NO2 and on what is the proportion of the abatement of pollution directly related to the lockdown, without meteorological interferences. ; The present work was supported by the Spanish Ministry of Agriculture, Fishing, Food and Environment, Madrid City Council and Madrid Regional Government, by the Ministry of Economy, Industry and Competitiveness and FEDER funds under the project HOUSE (CGL2016-78594-R), and by the Generalitat de Catalunya (AGAUR 2015 SGR33), and by the Spanish Ministry of Sciences, Innovation and Universities (EQC2018-004598-P). ; Peer reviewed

PM10 was collected during an EMEP winter campaign of 2017-2018 in two urban background sites in Barcelona (BCN) and Granada (GRA), two Mediterranean cities in the coast and inland, respectively. The concentrations of PM10, organic carbon (OC), elemental carbon (EC), and organic molecular tracer compounds such as hopanes, anhydro-saccharides, polycyclic aromatic hydrocarbon, and several biogenic and anthropogenic markers of secondary organic aerosols (SOA) were two times higher in GRA compared to BCN and related to the atmospheric mixing heights in the areas. Multivariate curve resolution (MCR-ALS) source apportionment analysis identified primary emissions sources (traffic + biomass burning) that were responsible for the 50% and 20% of the organic aerosol contributions in Granada and Barcelona, respectively. The contribution of biomass burning was higher in the holidays than in the working days in GRA while all primary combustion emissions decreased in holidays in BCN. The MCR-ALS identified that oxidative species and SOA formation processes contributed to 40% and 80% in Granada and Barcelona, respectively. Aged SOA was dominant in Granada and Barcelona under stagnant atmospheric conditions and in presence of air pollution. On the other hand, fresh SOA contributions from α-pinene oxidation (cis-pinonic acid) were three times higher in Barcelona than Granada and could be related to new particle formation, essentially due to overall cleaner air conditions and elevated air temperatures. ; Financial support for this study was provided by the Cooperative Programme for Monitoring and Evaluation of the Long-Range Transmission of Air Pollution in Europe (EMEP) and the European Union's Horizon 2020 research project ACTRIS2 (654109) and supported by research projects from the Plan Nacional de IyD of the Spanish Ministry of Science and Innovation INTEMPOL (PGC2018-102288-B-I00), HOUSE (CGL2016-78594-R), and BioCloud (RTI2018.101154.A.I00). IDAEA-CSIC is a Severo Ochoa Centre of Research Excellence (Spanish Ministry of Science and Innovation, CEX2018-000794-S). ; Peer reviewed

The present work assesses indoor air quality in stations of the Barcelona subway system. PM2.5 concentrations on the platforms of 4 subway stations were measured during two different seasons and the chemical composition was determined. A Positive Matrix Factorization analysis was performed to identify and quantify the contributions of major PM2.5 sources in the subway stations. Mean PM2.5 concentrations varied according to the stations design and seasonal periods. PM2.5 was composed of haematite, carbonaceous aerosol, crustal matter, secondary inorganic compounds, trace elements, insoluble sulphate and halite. Organic compounds such as PAHs, nicotine, levoglucosan and aromatic musk compounds were also identified. Subway PM2.5 source comprised emissions from rails, wheels, catenaries, brake pads and pantographs. The subway source showed different chemical profiles for each station, but was always dominated by Fe. Control actions on the source are important for the achievement of better air quality in the subway environment. © 2015 The Authors. ; The present study was supported by the European Union Seventh Framework Programme (FP7/2007-2013) under grant agreement no. 315760 HEXACOMM, the Spanish Ministry of Economy and Competitiveness and FEDER funds ( METRO CGL2012-33066 ), and the IMPROVE LIFE project ( LIFE13 ENV/ES/000263 ). Fulvio Amato is beneficiary of an AXA Research Fund postdoctoral grant. The authors would like to thank the Transports Metropolitans de Barcelona METRO staff who arranged the sampling campaign and contributed actively to this work. Appendix A ; Peer reviewed

Air quality in subway systems is of interest not only because particulate matter (PM) concentrations can be high, but also because of the peculiarly metalliferous chemical character of the particles, most of which differ radically from those of outdoor ambient air. We report on the oxidative potential (OP) of PM2.5 samples collected in the Barcelona subway system in different types of stations. The PM chemical composition of these samples showed typically high concentrations of Fe, Total Carbon, Ba, Cu, Mn, Zn and Cr sourced from rail tracks, wheels, catenaries, brake pads and pantographs. Two toxicological indicators of oxidative activity, ascorbic acid (AA) oxidation (expressed as OPAA μg−1 or OPAA m−3) and glutathione (GSH) oxidation (expressed as OPGSH μg−1 or OPGSH m−3), showed low OP for all samples (compared with outdoor air) but considerable variation between stations (0.9–2.4 OPAA μg−1; 0.4–1.9 OPGSH μg−1). Results indicate that subway PM toxicity is not related to variations in PM2.5 concentrations produced by ventilation changes, tunnel works, or station design, but may be affected more by the presence of metallic trace elements such as Cu and Sb sourced from brakes and pantographs. The OP assays employed do not reveal toxic effects from the highly ferruginous component present in subway dust. © 2016 The Authors ; This study was supported by the Spanish Ministry of Economy and Competitiveness and FEDER funds (METRO CGL2012-33066 ), the I MPROVE LIFE Project ( LIFE13 ENV/ES/000263 ) and the European Union Seventh Framework Programme ( FP7/2007-2013 ) under grant agreement no. 315760 HEXACOMM. Support is also acknowledged to Generalitat de Catalunya 2014 SGR33 . Fulvio Amato is beneficiary of an AXA Research Fund postdoctoral grant . In the UK the research was funded by the National Institute for Health Research Health Protection Research Unit (NIHR HPRU) in Health Impact of Environmental Hazards at King's College London in partnership with Public Health England (PHE). The views expressed are those of the authors and not necessarily those of the NHS, the NIHR, the Department of Health or Public Health England. Special thanks to Wes Gibbons for improving an early draft of the manuscript. Appendix A ; Peer reviewed

Access to detailed comparisons in air quality variations encountered when commuting through a city offers the urban traveller more informed choice on how to minimise personal exposure to inhalable pollutants. In this study we report on an experiment designed to compare atmospheric contaminants inhaled during bus, subway train, tram and walking journeys through the city of Barcelona. Average number concentrations of particles 10-300 nm in size, N, are lowest in the commute using subway trains (N5.0×104cm-3), with extreme transient peaks at busy traffic crossings commonly exceeding 1.0×105cm-3 and accompanied by peaks in Black Carbon and CO. Subway particles are coarser (mode 90nm) than in buses, trams or outdoors (1200ppm in crowded buses and trains. There are also striking differences in inhalable particle chemistry depending on the route chosen, ranging from aluminosiliceous at roadsides and near pavement works, ferruginous with enhanced Mn, Co, Zn, Sr and Ba in the subway environment, and higher levels of Sb and Cu inside the bus. We graphically display such chemical variations using a ternary diagram to emphasise how "air quality" in the city involves a consideration of both physical and chemical parameters, and is not simply a question of measuring particle number or mass. © 2015 The Authors. ; This work was supported by the ACS Foundation contributing to the dissemination of good environmental practices and environmental protection activities, the Spanish Ministry of Economy and Competitiveness and FEDER funds within the I+D Project CGL2012-33066 (METRO), and the IMPROVE LIFE project ( LIFE13 ENV/ES/000263 ). VM and ASF acknowledge funding from the European Union Seventh Framework Programme ( FP7/2007-2013 ) for a Marie Curie ITN (Grant agreement no. 315760 HEXACOMM ). Additional funding from AXA Research Fund is acknowledged. Fulvio Amato is beneficiary of the Juan de la Cierva postdoctoral Grant ( JCI-2012-13473 ) from the Spanish Ministry of Economy and Competitiveness. Appendix A ; Peer reviewed

Ground-level and vertical measurements (performed using tethered and non-tethered balloons), coupled with modelling, of ozone (O3), other gaseous pollutants (NO, NO2, CO, SO2) and aerosols were carried out in the plains (Vic Plain) and valleys of the northern region of the (BMA) in July 2015, an area typically recording the highest O3 episodes in Spain. Our results suggest that these very high O3 episodes were originated by three main contributions: (i) the surface fumigation from high O3 reservoir layers located at 1500-3000 mg-a.g.l. (according to modelling and non-tethered balloon measurements), and originated during the previous day(s) injections of polluted air masses at high altitude; (ii) local/regional photochemical production and transport (at lower heights) from the BMA and the surrounding coastal settlements, into the inland valleys; and (iii) external (to the study area) contributions of both O3 and precursors. These processes gave rise to maximal O3 levels in the inland plains and valleys northwards from the BMA when compared to the higher mountain sites. Thus, a maximum O3 concentration was observed within the lower tropospheric layer, characterised by an upward increase of O3 and black carbon (BC) up to around 100-200 m a.g.l. (reaching up to 300 μg mg-3 of O3 as a 10 s average), followed by a decrease of both pollutants at higher altitudes, where BC and O3 concentrations alternate in layers with parallel variations, probably as a consequence of the atmospheric transport from the BMA and the return flows (to the sea) of strata injected at certain heights the previous day(s). At the highest altitudes reached in this study with the tethered balloons (900-1000 m a.g.l.) during the campaign, BC and O3 were often anti-correlated or unrelated, possibly due to a prevailing regional or even hemispheric contribution of O3 at those altitudes. In the central hours of the days a homogeneous O3 distribution was evidenced for the lowest 1 km of the atmosphere, although probably important variations could be expected at higher levels, where the high O3 return strata are injected according to the modelling results and non-tethered balloon data. Relatively low concentrations of ultrafine particles (UFPs) were found during the study, and nucleation episodes were only detected in the boundary layer. Two types of O3 episodes were identified: type A with major exceedances of the O3 information threshold (180 μg mg-3 on an hourly basis) caused by a clear daily concatenation of local/regional production with accumulation (at upper levels), fumigation and direct transport from the BMA (closed circulation); and type B with regional O3 production without major recirculation (or fumigation) of the polluted BMA/regional air masses (open circulation), and relatively lower O3 levels, but still exceeding the 8 h averaged health target. To implement potential O3 control and abatement strategies two major key tasks are proposed: (i) meteorological forecasting, from June to August, to predict recirculation episodes so that NOx and VOC abatement measures can be applied before these episodes start; (ii) sensitivity analysis with high-resolution modelling to evaluate the effectiveness of these potential abatement measures of precursors for O3 reduction. © 2017 Author(s). ; The present work was supported by the Spanish Ministry of Economy and Competitiveness and FEDER funds under the project HOUSE (CGL2016-78594-R), by the Generalitat de Catalunya (AGAUR 2015 SGR33 and the DGQA). Part of this research was supported by the Korean Ministry of the Environment through "The Eco-Innovation project". The participation of University of Marseille and University of Birmingham was partially supported by two TNA actions projects carried out under the ACTRIS2 project (grant agreement No. 654109) financed by the European Union's Horizon 2020 research and innovation program. The support of the CUD of Zaragoza (project CUD 2013-18) is also acknowledged. We are very thankful to the Generalitat de Catalunya for supplying the air quality data from the XVPCA stations, to METEOCAT (the Meteorological Office of Catalonia) for providing meteorological data and to the IES J. Callís and the Meteorological Station from Vica (especially to Manel Dot) for allowing the performance of the vertical profiles and mobile unit measurements, respectively. In memoriam of Andrei Lyasota ; Peer reviewed

The vertical profile of new particle formation (NPF) events was studied by comparing the aerosol size number distributions measured aloft and at surface level in a suburban environment in Madrid, Spain, using airborne instruments. The horizontal distribution and regional impact of the NPF events was investigated with data from three urban, urban background, and suburban stations in the Madrid metropolitan area. Intensive regional NPF episodes followed by particle growth were simultaneously recorded at three stations in and around Madrid during a field campaign in July 2016. The urban stations presented larger formation rates compared to the suburban station. Condensation and coagulation sinks followed a similar evolution at all stations, with higher values at urban stations. However, the total number concentration of particles larger than 2.5 nm was lower at the urban station and peaked around noon, when black carbon (BC) levels are at a minimum. The vertical soundings demonstrated that ultrafine particles (UFPs) are formed exclusively inside the mixed layer. As convection becomes more effective and the mixed layer grows, UFPs are detected at higher levels. The morning soundings revealed the presence of a residual layer in the upper levels in which aged particles (nucleated and grown on previous days) prevail. The particles in this layer also grow in size, with growth rates significantly smaller than those inside the mixed layer. Under conditions with strong enough convection, the soundings revealed homogeneous number size distributions and growth rates at all altitudes, which follow the same evolution at the other stations considered in this study. This indicates that UFPs are detected quasi-homogenously in an area spanning at least 17 km horizontally. The NPF events extend over the full vertical extension of the mixed layer, which can reach as high as 3000 m in the area, according to previous studies. On some days a marked decline in particle size (shrinkage) was observed in the afternoon, associated with a change in air masses. Additionally, a few nocturnal nucleation-mode bursts were observed at the urban stations, for which further research is needed to elucidate their origin. © Author(s) 2018. ; This work was supported by the Spanish Ministry of Agriculture, Fishing, Food and Environment; the Ministry of Economy, Industry and Competitiveness; the Madrid City Council and Regional Government; FEDER funds under the project HOUSE (CGL2016-78594-R); the CUD of Zaragoza (project CUD 2016-05); the Government of Catalonia (AGAUR 2017 SGR44); and the Korean Ministry of Environment through "The Eco-Innovation project". The funding received by ERA-PLANET (http://www.era-planet.eu, last access: 16 November 2018), the trans-national project SMURBS (http://www.smurbs.eu, last access: 16 November 2018) (Grant agreement No. 689443), and the support of the Academy of Finland via the Center of Excellence in Atmospheric Sciences are acknowledged. These results are part of a project (ATM-GTP/ERC) that has received funding from the European Research Council (ERC) under the European Union's Horizon 2020 research and innovation program (Grant agreement No. 742206). The authors also acknowledge the Doctoral program of Atmospheric Sciences at the University of Helsinki (ATM-DP). Markku Kulmala acknowledges the support of the Academy of Finland via his Academy Professorship (no. 302958). We also thank the City Council of Majadahonda for logistic assistance, and the Instituto de Ciencias Agrarias, Instituto de Salud Carlos III, Alava Ingenieros, TSI, Solma Environmental Solutions, and Airmodus for their support. ; Peer reviewed