Towards a better understanding of fine PM sources: Online and offline datasets combination in a single PMF.

Source apportionment (SA) techniques allocate the measured ambient pollutants with their potential source origin; thus, they are a powerful tool for designing air pollution mitigation strategies. Positive Matrix Factorization (PMF) is one of the most widely used SA approaches, and its multi-time resolution (MTR) methodology, which enables mixing different instrument data in their original time resolution, was the focus of this study. One year of co-located measurements in Barcelona, Spain, of non-refractory submicronic particulate matter (NR-PM1), black carbon (BC) and metals were obtained by a Q-ACSM (Aerodyne Research Inc.), an aethalometer (Aerosol d.o.o.) and fine offline quartz-fibre filters, respectively. These data were combined in a MTR PMF analysis preserving the high time resolution (30 min for the NR-PM1 and BC, and 24 h every 4th day for the offline samples). The MTR-PMF outcomes were assessed varying the time resolution of the high-resolution data subset and exploring the error weightings of both subsets. The time resolution assessment revealed that averaging the high-resolution data was disadvantageous in terms of model residuals and environmental interpretability. The MTR-PMF resolved eight PM1 sources: ammonium sulphate + heavy oil combustion (25%), ammonium nitrate + ammonium chloride (17%), aged secondary organic aerosol (SOA) (16%), traffic (14%), biomass burning (9%), fresh SOA (8%), cooking-like organic aerosol (5%), and industry (4%). The MTR-PMF technique identified two more sources relative to the 24 h base case data subset using the same species and four more with respect to the pseudo-conventional approach mimicking offline PMF, indicating that the combination of both high and low TR data is significantly beneficial for SA. Besides the higher number of sources, the MTR-PMF technique has enabled some sources disentanglement compared to the pseudo-conventional and base case PMF as well as the characterisation of their intra-day patterns.

How can ventilation be improved on public transportation buses? Insights from CO2 measurements.

Measurements of CO2 and counting of occupants were carried out in 37 public bus trips during commuting rush hours in Barcelona (NE Spain) with the aim of evaluating parameters governing ventilation inside the vehicles and proposing actions to improve it. The results show that CO2 concentrations (1039 and 934 ± 386 ppm, as average and median, during rush hours but with average reduced occupancy due to the fair to be infected by SARS-CoV-2 during the measurement period, and measured in the middle of the busses) are in the lower range of values recorded in the literature for public buses, however an improvement in ventilation is required in a significant proportion of the journeys. Thus, we found better ventilation in the older Euro 3+ (retrofitted with filter traps and selective catalytic reduction) and Euro 5 buses (average 918 ± 257 ppm) than in the hermetically closed new Euro 6 ones (1111 ± 432 ppm). The opening of the windows in the older buses yielded higher ventilation rates (778 ± 432 ppm). The opening of all doors at all stops increases the ventilation by causing a fall in concentrations of 200-350 ppm below inter-stop concentrations, with this effect typically lasting 40-50 s in the hermetically closed new Euro 6 hybrid buses. Based on these results a number of recommendations are offered in order to improve ventilation, including measurement of CO2 and occupancy, and installation of ventilation fans on the top of the hermetically closed new buses, introducing outdoor air when a given concentration threshold is exceeded. In these cases, a CO2 sensor installed in the outdoor air intake is also recommended to take into account external CO2 contributions.

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.

Tracing surface and airborne SARS-CoV-2 RNA inside public buses and subway trains.

Given the widespread concern but general lack of information over the possibility of SARS-CoV-2 infection in public transport, key issues such as passenger personal hygiene, efficient air circulation systems, and the effective disinfection of frequently touched surfaces need to be evaluated to educate the public and diminish the risk of viral transmission as we learn to live with the ongoing pandemic. In this context we report on a study involving the collection of 99 samples taken from inside Barcelona buses and subway trains in May to July 2020. From this sample group 82 (58 surface swabs, 9 air conditioning (a/c) filters, 3 a/c dust, 12 ambient air) were selected to be analysed by RT-PCR for traces of the SARS-CoV-2 virus. Thirty of these selected samples showed evidence for one or more of 3 target RNA gene regions specific for this virus (IP2, IP4, E). Most (24) of these 30 samples showed positivity for only 1 of the 3 RNA targets, 4 samples yielded 2 targets, and 2 samples provided evidence for all 3 targets. RNA remnants were more common in surface swabs from support bars (23 out of 58) than in ambient air inside the vehicles (3 out of 12), with relatively higher concentrations of viral RNA fragments in buses rather than in trains. Whereas subway train a/c filters examined were all virus-free, 4 of the 9 bus a/c filter/dust samples yielded evidence for viral RNA. After nocturnal maintenance and cleaning most buses initially yielding positive results subsequently showed elimination of the RT-PCR signal, although signs of viral RNA remained in 4 of 13 initially positive samples. The presence of such remnant viral traces however does not demonstrate infectivity, which in the present study is considered unlikely given the fragmentary nature of the gene targets detected. Nevertheless, best practice demands that close attention to ventilation systems and regular vehicle disinfection in public transport worldwide need to be rigorously applied to be effective at eliminating traces of the virus throughout the vehicle, especially at times when COVID-19 cases are peaking. Additionally, infectivity tests should be implemented to evaluate the efficiency of disinfection procedures to complement the information resulting from RT-PCR analysis. Modelling the probability of infection whilst travelling in buses under different scenarios indicates that forced ventilation greatly reduces the risk.

Changes in air quality during the lockdown in Barcelona (Spain) one month into the SARS-CoV-2 epidemic.

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.

Source apportionment of urban PM1 in Barcelona during SAPUSS using organic and inorganic components.

Source apportionment of atmospheric PM1 is important for air quality control, especially in urban areas where high mass concentrations are often observed. Chemical analysis of molecular inorganic and organic tracer compounds and subsequently data analysis with receptor models give insight on the origin of the PM1 sources. In the present study, four source apportionment approaches were compared with an extended database containing inorganic and organic compounds that were measured during an intensive sampling campaign at urban traffic and urban background sites in Barcelona. Source apportionment of the combined database, containing both inorganic and organic compounds, was compared with more conventional approaches using inorganic and organic databases separately. Traffic emission sources were identified in all models for the two sites. The combined inorganic and organic databases provided higher discrimination capacity of emission sources. It identified aerosols generated by regional recirculation of biomass burning, secondary biogenic organic aerosols, harbor emissions, and specific industrial emissions. In this respect, this approach identified a relevant industrial source situated at NE Barcelona in which a waste incinerator plant, a combined-cycle power plant, and an industrial glass complex are located. Models using both inorganic and organic molecular tracer compounds improve the source apportionment of urban PM.

On the Relationship between Exposure to Particles and Dustiness during Handling of Powders in Industrial Settings.

Exposure to ceramic powders, which is frequent during handling operations, is known to cause adverse health effects. Finding proxy parameters to quantify exposure is useful for efficient and timely exposure assessments. Worker exposure during handling of five materials [a silica sand (SI1), three quartzes (Q1, Q2, and Q3), and a kaolin (K1)] with different particle shape (prismatic and platy) and sizes (3.4-120 µm) was assessed. Materials handling was simulated using a dry pendular mill under two different energy settings (low and high). Three repetitions of two kilos of material were carried out per material and energy conditions with a flow rate of 8-11 kg h-1. The performance of the dustiness index as a predictor of worker exposure was evaluated correlating material's dustiness indexes (with rotating drum and continuous drop) with exposure concentrations. Significant impacts on worker exposure in terms of inhalable and respirable mass fractions were detected for all materials. Mean inhalable mass concentrations during background were always lower than 40 µg m-3 whereas during material handling under high energy settings mean concentrations were 187, 373, 243, 156, and 430 µg m-3 for SI1, Q1, Q2, Q3, and K1, respectively. Impacts were not significant with regard to particle number concentration: background particle number concentrations ranged between 10 620 and 46 421 cm-3 while during handling under high energy settings they were 20 880 - 40 498 cm-3. Mean lung deposited surface area during background ranged between 27 and 101 µm2 cm-3 whereas it ranged between 22 and 42 µm2 cm-3 during materials handling. TEM images evidenced the presence of nanoparticles (≤100 nm) in the form of aggregates (300 nm-1 µm) in the worker area, and a slight reduction on mean particle size during handling was detected. Dustiness and exposure concentrations showed a high degree of correlation (R2 = 0.77-0.97) for the materials and operating conditions assessed, suggesting that dustiness could be considered a relevant predictor for workplace exposure. Nevertheless, the relationship between dustiness and exposure is complex and should be assessed for each process, taking into account not only material behaviour but also energy settings and workplace characteristics.

The effect of ventilation protocols on airborne particulate matter in subway systems.

As part of the European-funded IMPROVE LIFE project work programme experiments were performed in the Barcelona Metro system with the objective of better understanding the relationship between ventilation and air quality. The results demonstrate that tunnel ventilation plays an extremely important role in maintaining cleaner air and is capable of reducing both inhalable particulate matter (PM) mass and particle number concentration (>0.3µm) on platforms by over 50%, even in the presence of full-length platform screen doors. Another key influence on platform air quality is the chosen combination of fan power and forced air flow direction (impulsion of outdoor ambient air or extraction of subway indoor air): cleaner platform air was achieved using platform impulsion at higher power settings designed to ameliorate high summer temperatures underground. Reversing platform air flow from impulsion to extraction produced an immediate deterioration in PM air quality, most notably if the higher power setting was maintained, when an especially marked increase in numbers of very fine (submicron) particles was observed and attributed to tunnel air being drawn into the platform. At night, in the absence of trains and platform ventilation, platform air quality improves when tunnel fans are working at reduced power, whatever the flow direction (impulsion/extraction). Inside the air conditioned Barcelona Metro trains (where underground commuters spend most of their time) air quality is markedly better than on the platform, and unchanged A/C filters were observed capable of maintaining a similar reduction in inside train PM for at least three months.

Factors controlling air quality in different European subway systems.

Sampling campaigns using the same equipment and methodology were conducted to assess and compare the air quality at three South European subway systems (Barcelona, Athens and Oporto), focusing on concentrations and chemical composition of PM2.5 on subway platforms, as well as PM2.5 concentrations inside trains. Experimental results showed that the mean PM2.5 concentrations widely varied among the European subway systems, and even among different platforms within the same underground system, which might be associated to distinct station and tunnel designs and ventilation systems. In all cases PM2.5 concentrations on the platforms were higher than those in the urban ambient air, evidencing that there is generation of PM2.5 associated with the subway systems operation. Subway PM2.5 consisted of elemental iron, total carbon, crustal matter, secondary inorganic compounds, insoluble sulphate, halite and trace elements. Of all metals, Fe was the most abundant, accounting for 29-43% of the total PM2.5 mass (41-61% if Fe2O3 is considered), indicating the existence of an Fe source in the subway system, which could have its origin in mechanical friction and wear processes between rails, wheels and brakes. The trace elements with the highest enrichment in the subway PM2.5 were Ba, Cu, Mn, Zn, Cr, Sb, Sr, Ni, Sn, Co, Zr and Mo. Similar PM2.5 diurnal trends were observed on platforms from different subway systems, with higher concentrations during subway operating hours than during the transport service interruption, and lower levels on weekends than on weekdays. PM2.5 concentrations depended largely on the operation and frequency of the trains and the ventilation system, and were lower inside the trains, when air conditioning system was operating properly, than on the platforms. However, the PM2.5 concentrations increased considerably when the train windows were open. The PM2.5 levels inside the trains decreased with the trains passage in aboveground sections.

Origin of inorganic and organic components of PM2.5 in subway stations of Barcelona, Spain.

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.

Exposure to airborne particulate matter in the subway system.

The Barcelona subway system comprises eight subway lines, at different depths, with different tunnel dimensions, station designs and train frequencies. An extensive measurement campaign was performed in this subway system in order to characterise the airborne particulate matter (PM) measuring its concentration and investigating its variability, both inside trains and on platforms, in two different seasonal periods (warmer and colder), to better understand the main factors controlling it, and therefore the way to improve air quality. The majority of PM in the underground stations is generated within the subway system, due to abrasion and wear of rail tracks, wheels and braking pads caused during the motion of the trains. Substantial variation in average PM concentrations between underground stations was observed, which might be associated to different ventilation and air conditioning systems, characteristics/design of each station and variations in the train frequency. Average PM2.5 concentrations on the platforms in the subway operating hours ranged from 20 to 51 and from 41 to 91 µg m(-3) in the warmer and colder period, respectively, mainly related to the seasonal changes in the subway ventilation systems. The new subway lines with platform screen doors showed PM2.5 concentrations lower than those in the conventional system, which is probably attributable not only to the more advanced ventilation setup, but also to the lower train frequency and the design of the stations. PM concentrations inside the trains were generally lower than those on the platforms, which is attributable to the air conditioning systems operating inside the trains, which are equipped with air filters. This study allows the analysis and quantification of the impact of different ventilation settings on air quality, which provides an improvement on the knowledge for the general understanding and good management of air quality in the subway system.

PM10 concentration in urban atmosphere around the eastern Tien Shan, Central Asia during 2007-2013.

Based on the daily records from 16 cities around the eastern Tien Shan (Tianshan Mountains), central Asia from 2007 to 2013, the spatial pattern and seasonal/interannual variation of urban particulate matter up to 10 µm in size (PM10) concentrations and influencing factors were analyzed. Annual mean PM10 concentrations (±standard deviation) in most cities on the northern slope mainly range from 55 ± 28 µg/m(3) to 92 ± 75 µg/m(3), and those on the southern slope range between 96 ± 65 and 195 ± 144 µg/m(3). PM10 concentrations are maxima in winter on the northern slope, while they maximize in springtime on the southern slope. There is an increasing trend in annual mean concentrations during the period 2007-2013, which is not statistically significant at the 0.05 level. Urban PM10 concentration in the study region is jointly influenced by anthropogenic emission and regional natural processes, especially dust events and precipitation. The northern slope usually has heavy anthropogenic air pollution (mostly in winter) and relatively rich precipitation especially in summer, and the southern slope always suffers more frequent dust events (mostly in spring) and less precipitation. Modeled back-trajectory indicated that the Taklimakan desert source can greatly increase the PM10 concentration on the southern slope, and the mountain ranges may hinder the transport of dust to the northern slope.

A new look at inhalable metalliferous airborne particles on rail subway platforms.

Most particles breathed on rail subway platforms are highly ferruginous (FePM) and extremely small (nanometric to a few microns in size). High magnification observations of particle texture and chemistry on airborne PM10 samples collected from the Barcelona Metro, combined with published experimental work on particle generation by frictional sliding, allow us to propose a general model to explain the origin of most subway FePM. Particle generation occurs by mechanical wear at the brake-wheel and wheel-rail interfaces, where magnetic metallic flakes and splinters are released and undergo progressive atmospheric oxidation from metallic iron to magnetite and maghemite. Flakes of magnetite typically comprise mottled mosaics of octahedral nanocrystals (10-20 nm) that become pseudomorphed by maghemite. Continued oxidation results in extensive alteration of the magnetic nanostructure to more rounded aggregates of non-magnetic hematite nanocrystals, with magnetic precursors (including iron metal) still preserved in some particle cores. Particles derived from steel wheel and rails contain a characteristic trace element chemistry, typically with Mn/Fe=0.01. Flakes released from brakes are chemically very distinctive, depending on the pad composition, being always carbonaceous, commonly barium-rich, and texturally inhomogeneous, with trace elements present in nanominerals incorporated within the crystalline structure. In the studied subway lines of Barcelona at least there appears to be only a minimal aerosol contribution from high temperature processes such as sparking. To date there is no strong evidence that these chemically and texturally complex inhalable metallic materials are any more or less toxic than street-level urban particles, and as with outdoor air, the priority in subway air quality should be to reduce high mass concentrations of aerosol present in some stations.

Particulate air pollution and preeclampsia: a source-based analysis.

OBJECTIVES: To investigate the association between preeclampsia and maternal exposure to ambient particulate matter (PM) with aerodynamic diameter less than 10 µm (PM10) and 2.5 µm (PM2.5) mass and sources. METHODS: Our analysis was based on a hospital cohort of pregnant women (N=3182) residing in Barcelona, Spain, during 2003-2005. Positive matrix factorisation source apportionment (PMF2) was used to identify sources of PM10 and PM2.5 samples obtained by an urban background monitor, resulting in detection of eight sources. We further combined traffic-related sources (brake dust, vehicle exhaust and secondary nitrate/organics) to generate an indicator of combined traffic sources. Logistic regression models were developed to estimate the association between preeclampsia and exposure to each PM source and mass separately during the entire pregnancy and trimester one, adjusted for relevant covariates. RESULTS: For the exposure during the entire pregnancy, we found a 44% (95% CI 7% to 94%) and a 80% (95% CI 4% to 211%) increase in the risk of preeclampsia associated with one IQR increase in exposure to PM10 brake dust and combined traffic-related sources, respectively. These findings remained consistent after an alternative source apportionment method (Multilinear Engine (ME2)) was used. The results for PM2.5 mass and sources and also exposure during trimester one were inconclusive. CONCLUSIONS: Risk of preeclampsia was associated with exposure to PM10 brake dust and combined traffic-related sources.

Application of optimally scaled target factor analysis for assessing source contribution of ambient PM10.

Speciated coarse particulate matter (PM10) data obtained at three air quality monitoring sites in a highly industrialized area in Spain between 2002 and 2007 were analyzed for assessing source contribution of ambient particulate matter (PM). The source apportionment of PM in this area is an especially difficult task. There are industrial mineral dust emissions that need to be separately quantified from the natural sources of mineral PM. On the other hand, the diversity of industrial processes in the area results in a puzzling industrial emissions scenario. To solve this complex problem, a two-step methodology based on the possibilities of the Multilinear Engine was used. Application of positive matrix factorization to the dataset allowed the identification of nine factors relevant to the study area. This preliminary analysis permitted resolving two mineral factors. As a second step, a target rotation was implemented for transforming the mineral factors into experimentally characterized soil resuspension and industrial clay sources. In addition to improving the physical interpretation of these factors, the target rotation reduced the errors arising from the rotational freedom of the solution and the multicollinearity among sources. In this way, the main primary industrial emissions of PM in the zone were identified by this target factor analysis. A marked decrease was observed between 2002 and 2007 for the contributions of industrial sources coinciding with the implementation of mitigation measures in their processes. This study supports the utility of source apportionment methodologies for quantitatively evaluating the effectiveness of the abatement programs for air quality improvement.

Effect of ceramic industrial particulate emission control on key components of ambient PM10.

The relationship between specific particulate emission control and ambient levels of some PM(10) components (Zn, As, Pb, Cs, Tl) was evaluated. To this end, the industrial area of Castellón (Eastern Spain) was selected, where around 40% of the EU glazed ceramic tiles and a high proportion of EU ceramic frits are produced. The PM(10) emissions from the ceramic processes were calculated over the period 2000-2006, taking into account the degree of implementation of corrective measures throughout the study period. Abatement systems were implemented in the majority of the fusion kilns for frit manufacture in the area as a result of the application of the Directive 1996/61/EC, leading to a marked decrease in PM(10) emissions. By contrast, emissions from tile manufacture remained relatively constant because of the few changes in the implementation of corrective measures. On the other hand, ambient PM(10) levels and composition measurements were carried out from 2002 to 2006. A high correlation between PM(10) emissions from frit manufacture and ambient levels of Zn, As, Pb and Cs (R(2) from 0.61 to 0.98) was observed. On the basis of these results, the potential impact of the implementation of corrective measures to reduce emissions from tile manufacture was quantified, resulting in a possible decrease of 3-5 microg/m(3) and 2 microg/m(3) in ambient mineral PM(10) (on an annual basis) in urban and suburban areas, respectively. This relatively simple methodology allows us to estimate the direct effect of a reduction in primary particulate emissions on ambient levels of key particulate components, and to make a preliminary quantification of the possibilities of air quality improvement by means of further emission reduction. Therefore, it is a useful tool for developing future air quality plans in the study area and in other industrialised areas.

Lanthanoid geochemistry of urban atmospheric particulate matter.

Relatively little is known about the lanthanoid element (La to Lu) chemistry of inhalable urban atmospheric particulate matter (PM). PM samples collected during an air sampling campaign in the Mexico City area contain lanthanoid concentrations of mostly 1-10 ng m(-3), increasing with mass where resuspension of crustal PM is important (low PM2.5/PM10), but not where fine emissions from traffic and industry dominate (high PM2.5/ PM10). Samples show anthropogenic enrichment of lighter over heavier lanthanoids, and Ce enrichment relative to La and Sm occurs in the city center (especially PM10) possibly due to PM from road vehicle catalytic converters. La is especially enriched, although many samples show low La/V values (< 0.11), suggesting the dominating influence of fuel oil combustion sources rather than refinery emissions. We use La/Sm v La/ Ce, LaCeSm, and LaCeV plots to compare Mexico City aerosols with PM from other cities. Lanthanoid aerosol geochemistry can be used not only to identify refinery pollution events, but also as a marker for different hydrocarbon combustion emissions (e.g., oil or coal power stations) on urban background atmospheric PM.