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Background: The implementation of emission mitigation policies in Europe over the last two decades has generally improved the air quality, which resulted in lower aerosol particle mass, particle number, and black carbon mass concentration. However, little is known whether the decreasing particle concentrations at a lower-altitude level can be observed in the free troposphere (FT), an important layer of the atmosphere, where aerosol particles have a longer lifetime and may affect climate dynamics. In this study, we used data from two high-Alpine observatories, Zugspitze-Schneefernerhaus (ZSF) and Jungfraujoch (JFJ), to assess the long-term trends on size-resolved particle number concentrations (PNCs) and equivalent black carbon (eBC) mass concentration separated for undisturbed lower FT conditions and under the influence of air from the planetary boundary layer (PBL) from 2009 to 2018. Results: The FT and PBL-influenced conditions were segregated for both sites. We found that the FT conditions in cold months were more prevalent than in warm months, while the measured aerosol parameters showed different seasonal patterns for the FT and PBL-influenced conditions. The pollutants in the PBL-influenced condition have a higher chance to be transported to high-altitudes due to the mountainous topography, leading to a higher concentration and more distinct seasonal variation, and vice versa. The long-term trends of the measured aerosol parameters were evaluated and the decreased aerosol concentrations were observed for both FT and PBL-influenced conditions. The observed decreasing trends in eBC concentration in the PBL-influenced condition are well consistent with the reported trends in total BC emission in Germany and Switzerland. The decreased concentrations in the FT condition suggest that the background aerosol concentration in the lower FT over Central Europe has correspondingly decreased. The change of back trajectories in the FT condition at ZSF and JFJ was further evaluated to investigate the other possible drivers for the decreasing trends. Conclusions: The background aerosol concentration in the lower FT over Central Europe has significantly decreased during 2009–2018. The implementation of emission mitigation policies is the most decisive factor and the decrease of the regional airmass occurrence over Central Europe also has contributed to the decreasing trends. [ABSTRACT FROM AUTHOR]

Can mitigating only particle mass, as the existing air quality measures do, ultimately lead to reduction in ultrafine particles (UFP)? The aim of this study was to provide a broader urban perspective on the relationship between UFP, measured in terms of particle number concentration (PNC) and PM 2.5 (mass concentration of particles with aerodynamic diameter < 2.5 μm) and factors that influence their concentrations. Hourly average PNC and PM 2.5 were acquired from 10 cities located in North America, Europe, Asia, and Australia over a 12-month period. A pairwise comparison of the mean difference and the Kolmogorov-Smirnov test with the application of bootstrapping were performed for each city. Diurnal and seasonal trends were obtained using a generalized additive model (GAM). The particle number to mass concentration ratios and the Pearson's correlation coefficient were calculated to elucidate the nature of the relationship between these two metrics. Results show that the annual mean concentrations ranged from 8.0 × 103 to 19.5 × 103 particles·cm−3 and from 7.0 to 65.8 μg·m−3 for PNC and PM 2.5 , respectively, with the data distributions generally skewed to the right, and with a wider spread for PNC. PNC showed a more distinct diurnal trend compared with PM 2.5 , attributed to the high contributions of UFP from vehicular emissions to PNC. The variation in both PNC and PM 2.5 due to seasonality is linked to the cities' geographical location and features. Clustering the cities based on annual median concentrations of both PNC and PM 2.5 demonstrated that a high PNC level does not lead to a high PM 2.5 , and vice versa. The particle number-to-mass ratio (in units of 109 particles·μg−1) ranged from 0.14 to 2.2, >1 for roadside sites and <1 for urban background sites with lower values for more polluted cities. The Pearson's r ranged from 0.09 to 0.64 for the log-transformed data, indicating generally poor linear correlation between PNC and PM 2.5. Therefore, PNC and PM 2.5 measurements are not representative of each other; and regulating PM 2.5 does little to reduce PNC. This highlights the need to establish regulatory approaches and control measures to address the impacts of elevated UFP concentrations, especially in urban areas, considering their potential health risks. [ABSTRACT FROM AUTHOR]

Background: Particulate matter air pollution has been associated with adverse health effects. The fraction of ambient particles that are mainly responsible for the observed health effects is still a matter of controversy. Better characterization of the health relevant particle fraction will have major implications for air quality policy since it will determine which sources should be controlled. The RUPIOH study, an EU-funded multicentre study, was designed to examine the distribution of various ambient particle metrics in four European cities (Amsterdam, Athens, Birmingham, Helsinki) and assess their health effects in participants with asthma or COPD, based on a detailed exposure assessment. In this paper the association of central site measurements with respiratory symptoms and restriction of activities is examined. Methods: At each centre a panel of participants with either asthma or COPD recorded respiratory symptoms and restriction of activities in a diary for six months. Exposure assessment included simultaneous measurements of coarse, fine and ultrafine particles at a central site. Data on gaseous pollutants were also collected. The associations of the 24-hour average concentrations of air pollution indices with the health outcomes were assessed in a hierarchical modelling approach. A city specific analysis controlling for potential confounders was followed by a meta-analysis to provide overall effect estimates. Results: A 10 µg/m3 increase in previous day coarse particles concentrations was positively associated with most symptoms (an increase of 0.6 to 0.7% in average) and limitation in walking (OR= 1.076, 95% CI: 1.026-1.128). Same day, previous day and previous two days ozone concentrations were positively associated with cough (OR= 1.061, 95% CI: 1.013-1.111; OR= 1.049, 95% CI: 1.016-1.083 and OR= 1.059, 95% CI: 1.027-1.091, respectively). No consistent associations were observed between fine particle concentrations, nitrogen dioxide and respiratory health effects. As for particle number concentrations negative association (mostly non-significant at the nominal level) was observed with most symptoms whilst the positive association with limitation of activities did not reach the nominal level of significance. Conclusions: The observed associations with coarse particles are in agreement with the findings of toxicological studies. Together they suggest it is prudent to regulate also coarse particles in addition to fine particles. [ABSTRACT FROM AUTHOR]

Abstract: The number of ultrafine particles in urban air may be more health relevant than the usually measured mass of particles smaller than 2.5 or 10μm. Epidemiological studies typically assess exposure by measurements at a central site. Limited information is available about how well measurements at a central site reflect exposure to ultrafine particles. The goals of this paper are to assess the relationships between particle number (PN) and mass concentrations measured outdoors at a central site, right outside and inside the study homes. The study was conducted in four European cities: Amsterdam, Athens, Birmingham and Helsinki. Particle mass (PM10 and PM2.5), PN, soot and sulfate concentrations were measured at these sites. Measurements of indoors and outdoors near the home were made during 1 week in 152, mostly non-smoking, homes. In each city continuous measurements were also performed at a central site during the entire study period. The correlation between 24-h average central site outdoor and indoor concentrations was lower for PN (correlation among cities ranged from 0.18 to 0.45) than for PM2.5 (0.40–0.80), soot (0.64–0.92) and sulfate (0.91–0.99). In Athens, the indoor–central site correlation was similar for PN and PM2.5. Infiltration factors for PN and PM2.5 were lower than for sulfate and soot. Night-time hourly average PN concentrations showed higher correlations between indoor and central site, implying that indoor sources explained part of the low correlation found for 24-h average concentrations. Measurements at a central site may characterize indoor exposure to ambient particles less well for ultrafine particles than for fine particle mass, soot and sulfate. [Copyright &y& Elsevier]

The number of ultrafine particles may be a more health relevant characteristic of ambient particulate matter than the conventionally measured mass. Epidemiological time series studies typically use a central site to characterize human exposure to outdoor air pollution. There is currently very limited information how well measurements at a central site reflect temporal and spatial variation across an urban area for particle number concentrations (PNC). The main objective of the study was to assess the spatial variation of PNC compared to the mass concentration of particles with diameter less than 10 or 2.5μm (PM10 and PM2.5). Continuous measurements of PM10, PM2.5, PNC and soot concentrations were conducted at a central site during October 2002–March 2004 in four cities spread over Europe (Amsterdam, Athens, Birmingham and Helsinki). The same measurements were conducted directly outside 152 homes spread over the metropolitan areas. Each home was monitored during 1 week. We assessed the temporal correlation and the variability of absolute concentrations. For all particle indices, including particle number, temporal correlation of 24-h average concentrations was high. The median correlation for PNC per city ranged between 0.67 and 0.76. For PM2.5 median correlation ranged between 0.79 and 0.98. The median correlation for hourly average PNC was lower (range 0.56–0.66). Absolute concentration levels varied substantially more within cities for PNC and coarse particles than for PM2.5. Measurements at the central site reflected the temporal variation of 24-h average concentrations for all particle indices at the selected homes across the urban area. A central site could not assess absolute concentrations across the urban areas for particle number. [Copyright &y& Elsevier]