The use of a diffusion charger based AQ Urban sensors to monitor particle number concentrations was investigated in Helsinki metropolitan area. The comparisons between the AQ Urban sensors and traditional butanol CPCs were made at a heavily trafficked street canyon (Traffic Supersite) and at an urban background site (UB Supersite) in 2022. The agreement with the measured particle number concentrations within different AQ Urban units was good. Comparison of the AQ Urban sensor with the two CPCs showed that AQ Urban sensors should be suitable to measure concentration of particles approx. larger than 10 nm in highly trafficked areas. The long-term agreement between AQ Urban sensors and CPCs was also investigated in the two different environments between 1 January and 15 August 2022. Overall, the correlation between AQ Urban sensors and the CPCs was good at both sites (r being 0.93 and 0.89, respectively). The increased concentration of particles smaller than 10 nm and long-range transported pollution affected the accuracy of AQ Urban sensors. Despite this downside of the method, the correlation between the AQ Urban sensor and the CPCs was good during the whole measurement period, indicating that the sensor is well suitable for long-term particle number concentration monitoring in urban environments in Finland. However, the observed effect of bi-modal particle size distribution suggests that the performance of diffusion charger-based sensors may vary in different geographic regions depending on the regional background concentrations of accumulation mode particles which should be considered when applying the method in different locations.
Organic aerosol particles (OA) can absorb solar radiation with varying efficiencies depending on their chemical composition and physical properties. This light-absorbing fraction of OA, commonly referred to as brown carbon (BrC), is difficult to accurately represent in climate models due to the inherent diversity of its optical properties. This variability arises from differences in emission sources and atmospheric processing, as well as from variations in experimental design and the analytical methods used to quantify BrC absorption. As a result, the climate effect of BrC remains uncertain. Here, we studied the light absorption properties of surface ambient OA using measurements from 17 sites across Europe. Combining multi-wavelength absorption measurements from filter-based photometers with OA mass concentrations and source apportionment derived from ACSM/AMS data, we derive empirical estimates of the OA mass absorption cross section (MACOA), its wavelength dependence (AAEOA), the OA density (⍴OA), and the MAC associated with different primary and secondary OA sources. We further develop parameterizations that relate MACOA, AAEOA and ⍴OA to the ambient black carbon-to-organic aerosol ratio (eBC/OA) and propose a corresponding parameterization for the imaginary refractive index (kOA). Given the widespread availability of eBC and OA measurements in global monitoring networks, the framework presented here provides a practical approach for estimating the absorptive properties of surface OA particles under real-world conditions.
Recent studies suggest that terpenes in urban air may have substantial anthropogenic sources, yet distinguishing these from biogenic emissions remains challenging. In this study, we measured terpene concentrations in a street canyon in Helsinki during cold winter months (mean temperature < 0 °C), when biogenic emissions were expected to be minimal. Monoterpenes were observed at mean concentrations of ~160 ng m⁻³, more than an order of magnitude lower than the mixing ratios of aromatic hydrocarbons. Nevertheless, their high reactivity with hydroxyl radicals, nitrate radicals, and ozone led to a disproportionately large contribution to local atmospheric oxidation processes. This pronounced reactivity, combined with their high secondary organic aerosol (SOA) formation potential, indicated the important potential role of anthropogenic terpene emissions even in wintertime SOA formation.
This article presents the results of long-term air quality measurements (2015–2024) from the Helsinki Traffic Supersite, including gaseous compounds (NO, NO2, CO, CO2, O3), particulate matter (PM2.5, PM10, particle number (PN) and size distribution), chemical composition of PM (black carbon (BC), organic aerosol (OA), inorganic species), lung-deposited surface area (LDSA), polycyclic aromatic hydrocarbons, volatile organic compounds (VOC), as well as road surface conditions and meteorology. In addition to the long-term observations, large number of targeted short-term measurement campaigns were conducted to investigate emerging phenomena, to further develop supersite measurements and gain new information about sources impacting air quality.The observed air quality improvements at the Traffic Supersite were driven by declining traffic exhaust concentrations (NOx (-8.0%/yr), BC (-7.1%/yr), PN (-3.7%/yr), and anthropogenic VOCs (-3.1 to -8.9%/yr)). The observed emission factors (g/kgfuel) also decreased for NOx (-7.6%/yr), BC (-7.5%/yr), and PN (-4.1%/yr), reflecting fleet renewal. The observed rate of decrease in PN concentration was lower than that of other parameters, particularly in the smallest size classes (< 30 nm). Organic aerosol analysis showed that traffic hydrocarbon tracers (m/z 57) declined faster (-7.9%/yr) than total OA and oxidized OA (m/z 44), which are linked to secondary formation and long-range transport. Long-term results indicate that compliance with the upcoming EU Air Quality Directive limit values for 2030 is already largely achievable, with the most challenging aspect being the exceedances of the PM10 daily limit due to road dust events. However, achieving the EU Zero Pollution target for 2050 remains challenging, and the WHO guideline values for PM10, PM2.5 and NO2 continue to be exceeded. These unique findings highlight the importance of comprehensive, long-term supersite measurements for understanding pollutant sources and trends, and for supporting urban planning and policy development.
Carbonaceous aerosols (CA), composed of black carbon (BC) and organic matter (OM), significantly impact the climate. Light absorption properties of CA, particularly of BC and brown carbon (BrC), are crucial due to their contribution to global and regional warming. We present the absorption properties of BC (b(Abs,BC)) and BrC (b(Abs,BrC)) inferred using Aethalometer data from 44 European sites covering different environments (traffic (TR), urban (UB), suburban (SUB), regional background (RB) and mountain (M)). Absorption coefficients showed a clear relationship with station setting decreasing as follows: TR > UB > SUB > RB > M, with exceptions. The contribution of b(Abs,BrC) to total absorption (b(Abs)), i.e. %Abs(BrC), was lower at traffic sites (11-20 %), exceeding 30 % at some SUB and RB sites. Low AAE values were observed at TR sites, due to the dominance of internal combustion emissions, and at some remote RB/M sites, likely due to the lack of proximity to BrC sources, insufficient secondary processes generating BrC or the effect of photobleaching during transport. Higher b(Abs) and AAE were observed in Central/Eastern Europe compared to Western/Northern Europe, due to higher coal and biomass burning emissions in the east. Seasonal analysis showed increased b(Abs), b(Abs,BC), b(Abs,BrC) in winter, with stronger %Abs(BrC), leading to higher AAE. Diel cycles of b(Abs,BC) peaked during morning and evening rush hours, whereas b(Abs,BrC), %Abs(BrC), AAE, and AAE(BrC) peaked at night when emissions from household activities accumulated. Decade-long trends analyses demonstrated a decrease in b(Abs), due to reduction of BC emissions, while b(Abs,BrC) and AAE increased, suggesting a shift in CA composition, with a relative increase in BrC over BC. This study provides a unique dataset to assess the BrC effects on climate and confirms that BrC can contribute significantly to UV-VIS radiation presenting highly variable absorption properties in Europe.
Physical and chemical properties of particulate matter and concentrations of trace gases were measured at an urban site in Helsinki, Finland, for 5 weeks to investigate the effect of wintertime conditions on pollutants. The measurement took place in a street canyon (traffic supersite) in January–February 2022. In addition, measurements were conducted in an urban background station (UB supersite, SMEAR III, located approx. 0.9 km from the traffic supersite). Measurements were also made using the mobile laboratory. The measurements were made driving the adjacent side streets and the street along the traffic supersite. Source apportionment was performed for the soot particle aerosol mass spectrometer measurements to identify organic factors connected to different particulate sources. Particle number concentration time series and the pollution detection algorithm were used to compare local pollution level differences between the sites. During the campaign three different pollution events were observed with increased pollution concentrations. The increased concentrations during these episodes were due to both trapping of local pollutants near the boundary layer and the long-range and regional transport of pollutants to the Helsinki metropolitan area. Local road vehicle emissions increased the particle number concentrations, especially sub-10 nm particles, and long-range-transported and regionally transported aged particles increased the PM mass and particle size.
Accurate measurement of black carbon (BC) particles is vital for climate models as well as air quality assessments. While the need for BC particle measurement has been recognized, standardization of instruments and procedures for ambient measurement is still underway. In this study, we used laboratory generated soot particles to assess nine instruments targeting BC mass concentration measurement. The measurement matrix included different BC concentrations (ranging from atmospheric levels to combustion emission levels), different particle coatings, two particle sources (gas burner and spark generator) and two dilution methods. The nine instruments included six different models: aethalometers AE33 and MA200, thermo-optical OC-EC analysis, multi-angle absorption photometer MAAP 5012, photoacoustic instrument MSS, and soot particle aerosol mass spectrometer SP-AMS. The main discrepancy we observed was that the SP-AMS results were systematically lower, approximately only half of the BC measured by other instruments. A portion of this is explained by particle losses in the aerodynamic lens of the SP-AMS and the parameters used in the data analysis. Some smaller discrepancies were identified for the other instruments, but overall, the median values from were within 25 % of each other. Instruments’ operation principles and covered concentration ranges need to be carefully considered especially in emission measurements where the aerosols can have high temporal variation as well as high BC concentrations. In general, the results can decrease the uncertainties in climate and air quality studies by providing tools for more accurate and comparable BC measurements and when the existing BC data is interpreted.
It has become evident that additional metrics along the particle mass concentration, together with dense air quality monitoring networks within cities, are needed to understand the most efficient ways to tackle the health burden of particulate pollution. Particle lung-deposited surface area (LDSAal) is a metric to estimate particle exposure in the lung alveoli, and it has gained interest as a parameter for air quality monitoring as it is relatively easy and cost-efficient to measure with electrical particle sensors. Also, various studies have indicated its potential as a health-relevant metric. In addition to the electrical particle sensors, the LDSAal can be measured with various size distribution methods. However, different LDSAal measurement methods have fundamental differences in their operation principles, e.g., related to the measurement size ranges, size classification or conversion from the originally measured quantity into the LDSAal. It is not well understood how these differences affect the accuracy of the measurement in ambient conditions, where especially the particle effective density and hygroscopicity can considerably change the particle lung deposition efficiencies. In this study, the electrical particle sensor measurement (Partector) and two size distribution approaches (ELPI+ and DMPS/SMPS) were compared in road traffic environments with different environmental conditions in Helsinki and Prague. The results were compared by utilising the general assumptions of the LDSAal measurement (spherical hydrophobic particles with the standard density) and by evaluating the effects of the particle effective density and hygroscopicity. Additionally, the Partector and ELPI+ approaches were compared in various urban environments near road traffic, airports, river traffic and residential wood combustion. The results show that the comparison of different LDSAal measurement methods can be complicated in ambient measurements. The challenges were especially related to the accumulation mode particles roughly larger than 200–400 nm for which the dominant deposition mechanism in the lung changes from diffusion to impaction and the particle effective density and hygroscopicity tend to increase. On the other hand, the results suggest that the differences between the methods are reasonably low when considering only ultrafine and soot particles, which have an effective density closer to the standard (1.0 g cm−3) and are more hydrophobic, highlighting the suitability of the LDSAal as a monitored metric when estimating the spatial differences in the particulate pollution within cities.
Brown carbon (BrC) is an organic aerosol (OA) component that possesses light-absorbing properties in the UV-Vis spectrum, impacting climate. However, the current understanding of climate repercussions stemming from BrC emissions remains insufficient due to a lack of comprehensive knowledge regarding its chemical makeup, light-absorption, and the role of atmospheric aging in shaping BrC properties. This study investigates BrC in PM1 (particulate matter <1μm) during winter in Helsinki, Finland, in a street canyon and a residential area with wood combustion. The aim was to ascertain BrC sources, chemical composition, and contribution to UV-Vis light absorption. The study utilized a seven-wavelength aethalometer (AE33) to measure black carbon (BC) and BrC light absorptions, and a soot particle aerosol mass spectrometer (SP-AMS) to determine OA composition. An OA source apportionment using positive matrix factorization followed by a multiple regression analysis between BrC absorption and each factor was performed to determine the mass absorption coefficients of BrC (MACBrC) and light absorption contributions of distinct sources across 370-660 nm wavelengths. The BrC UV-Vis absorption relative to the one of BC was higher at 370 nm, with a median contribution of 20.1 % in the residential area and 18.2 % at the traffic site. Residential BrC absorption showed sporadic peaks, while street canyon absorption was lower but consistent. MACBrC was higher for biomass burning organic aerosol but still significant for long-range transported (LRT) and traffic-related aerosols. Hydrocarbon-like organic aerosol exhibited higher MACBrC at 470 nm than at 370 nm. Combined with particulate mass concentrations, biomass burning and LRT contributed the most to light absorption. Uncertainties regarding MACBrC were evaluated. The chemical composition analysis revealed stronger correlations between BrC absorption and SP-AMS-measured ions, especially in residential areas and for polycyclic aromatic hydrocarbons and oxidized aromatics. The study emphasizes the importance of anthropogenic sources in BrC light absorption.
The sources Sources and characteristics of particulate matter (PM) were determined in a modern underground chrome mine in Finland. Measurements were conducted at five locations in the mine: the maintenance area, blasting area, ore pit dumping area, crushing station and conveyor belt. The measurement set-up consisted of a Soot Particle Aerosol Mass Spectrometer (SP-AMS) for the particles’ chemical composition; an Electrical Low Pressure Impactor, Nano Scanning Mobility Particle Sizer and Optical Particle Counter for the particle number and mass size distribution; and an Aethalometer for black carbon (BC). The particle number and mass concentration depended strongly on the measurement location and period. The PM10 and the total number concentrations varied from 22 to 1100 μg m–3 and 1.7 × 103 to 2.3 × 105 # cm–3, respectively, in the mine. In terms of the composition, the sub-micrometer particles (PM1) consisted mostly of organic matter and BC, but at the blasting site, the fraction of sulfate was also significant. The SP-AMS data was analyzed with Positive Matrix Factorization (PMF) to identify and quantify the main sources of PM1 in the mine. Based on the PMF analysis, the PM1 originated mostly from diesel engines (35–84%) and blasting (7–60%). The impact of blasting on air quality in mines may become more pronounced in the future as the emissions from diesel engines decrease due to alternative fuels and better engine and after-treatment technologies.
The paper presents a novel technique for quantifying trace metals in aerosol samples in real time. Airborne metals were continuously collected for one week near the Baltic Sea in Finland using a particle-into-liquid sampler (PILS). The collected liquid samples were analyzed for metals using micro-discharge optical emission spectroscopy (µDOES). The micro-discharge analyzer is designed to perform real-time, on-site measurements of metal concentrations in aqueous solutions. Currently, µDOES can provide online measurements of 30 metals, with typical detection limits from 0.01 µg/m3 to 0.06 µg/m3 with a long-term repeatability less than 5
Atmospheric particulate matter samples (PM2.5 and PM10) were collected at urban sites (Sao Paulo, SPA; Piracicaba, PRB) in Sao Paulo State, Brazil. In order to characterize the chemical composition of particulate matter, several chemical components were analyzed from the samples, and among these were inorganic and organic anions, monosaccharide anhydrides, and organic and elemental carbon. Long-range transport of the particulate matter while sugar cane was being burned contributed to an increase in PM2.5 and PM10 concentrations at the SPA site. Sulphate, nitrate, ammonium, elemental carbon and particulate organic material (POM) were major components of the total PM2.5 and PM2.5-10. The contribution of POM to PM2.5 at PRB was 29%, similar to the results found for the winter season at the SPA site.The Cl-/Na+ ratio at the SPA site for PM2.5 was different from that at the other site, with chloride depletion indicating several sources beyond sea salt. The occurrence of levoglucosan and its correlations with potassium confirm the contribution of local biomass burning (at PRB) and long-range transported particles at SPA. OC/EC ratios and the correlation coefficients indicated secondary formation of OC at both sites.
Diesel engines contribute significantly to deteriorating air quality. Tightening legislation has led to various technological advances, but developments differ between countries. In India, air quality has not improved and fine particle (PM2.5) related premature deaths are predicted to increase. In this study, we characterized the particle emissions of an Indian-manufactured BS IV (Bharat Stage, comparable to Euro emission standards) heavy-duty diesel vehicle and studied the effects of different fuels, fuel blends and lubricating oils. The main aims of the study were to investigate the particle emission dependency on fuel types and fuel blends used in India and to produce useful data for further use (e.g. legislative parties and modeling): emission factors (PN, PM, BC, other chemical compounds), size distributions and volatility of particles. Additionally, the sensitivity of the emissions to the lubricating oil choice was studied. Two lubricating oils, two fossil fuels conforming to BS IV and BS VI emission standards and two biofuel – BS IV fossil fuel blends were tested, one containing Renewable Paraffinic Diesel (RPD) and the other renewable Fatty Acid Methyl Ester (r-FAME). The tests were conducted on a chassis dynamometer (Delhi Bus Driving Cycle, DBDC). Our results show that the emitted particles were in ultrafine particle size range, and both the soot mode particles and smaller nanoparticles were affected by fuels and lubricating oils. The transition from BS IV grade diesel to BSVI was shown to have potential in reducing particle emissions (PN and eBC) of heavy-duty diesel vehicles in India. Blending fossil fuel with biofuel strongly affected particle number emissions, chemical composition, and eBC emissions and the emissions were highly sensitive to biofuel type. Changing the lubricating oil had a comparable magnitude of effect as changing the fuel and the results indicate that in order to reduce particle emissions, a combination of fuel and lubricating oil should be chosen, instead of choosing them separately.
The chemical composition of PM2.5 was monitored simultaneously at two sites, one in a general area of the city center and one at a roadside, in Hanoi, Vietnam, during August 2019-July 2020 using 220 daily (24 h) filter samples. PM mass, water soluble ions, trace elements, organic and elemental carbon and sugar anhydrides were measured. The annual average PM2.5 concentrations, 49 and 46 mu g m(-3) at the traffic and the general urban site, respectively, exceeded the national (25 mu g m(-3)) and 2021 WHO limit values (5 mu g m(-3)). Daily PM2.5 concentrations were the highest in winter when stagnant meteorological conditions prevailed. On average, half of the resolved mass was organic matter, of which about 40% was attributable to biomass burning, most likely rice straw field burning and domestic fuel combustion. One third of PM2.5 was secondary inorganic aerosol which was dominated by sulphate hence indicating a high contribution of stationary sources like coal combustion. The elemental carbon level was higher at the traffic site, except in April 2020 during the COVID-19 restrictions. Zinc was the most common trace element with high daily variations and large differences between the sites, and it often peaked with Cd, Cl- and Pb indicating contribution of industrial sources and/or coal combustion. The highest zinc concentrations appeared on a few days and likely originated from open burning of municipal solid waste. It appeared that scattered open waste and biomass burning, as well as coal combustion, are important sources causing spikes of PM2.5 pollution in Hanoi above the general levels caused by routine industrial and traffic sources, especially during stagnant winter days. Source contributions were further studied with positive matrix factorization producing six source factors: traffic (12%), local secondary inorganic aerosol (SIA, 18%), biomass burning (19%), industry (9%), long-range transported SIA (25%) and dust (17%).
The differences in the traffic fuels have been shown to affect exhaust emissions and their toxicity. Especially, the aromatic content of diesel fuel is an important factor considering the emissions, notably particulate matter (PM) concentrations. The ultra-fine particles (UFP, particles with a diameter of <100 nm) are important components of engine emissions and connected to various health effects, such as pulmonary and systematic inflammation, and cardiovascular disorders. Studying the toxicity of the UFPs and how different fuel options can be used for mitigating the emissions and toxicity is crucial. In the present study, emissions from a heavy-duty diesel engine were used to assess the exhaust emission toxicity with a thermophoresis-based in vitro air-liquid interface (ALI) exposure system. The aim of the study was to evaluate the toxicity of engine exhaust and the potential effect of 20 % aromatic fossil diesel and 0 % aromatic renewable diesel fuel on emission toxicity. The results of the present study show that the aromatic content of the fuel increases emission toxicity, which was seen as an increase in genotoxicity, distinct inflammatory responses, and alterations in the cell cycle. The increase in genotoxicity was most likely due to the PM phase of the exhaust, as the exposures with high-efficiency particulate absorbing (HEPA)-filtered exhaust resulted in a negligible increase in genotoxicity. However, the solely gaseous exposures still elicited immunological responses. Overall, the present study shows that decreasing the aromatic content of the fuels could be a significant measure in mitigating traffic exhaust toxicity.
Elemental carbon (EC) and organic carbon (OC) are major components of atmospheric PM2.5. In this article we represent the results of long-term measurements (8-12 years) of EC and OC at three different background sites in Finland: in a rural area (Virolahti) since the summer 2010, in a marine environment (Uto & BULL;) since the summer 2011, and in a clean arctic environment (Pallas/Matorova) since 2014. The concentrations of OC and EC were measured with a semi-continuous organic and elemental carbon analyser (SC-OCEC) in all the sites. The yearly average concentrations of OC varied between 0.96-3.1, 0.76-1.6 and 0.30-0.69 & mu;g m 3 at the rural (Virolahti), marine (Uto & BULL;) and arctic (Pallas/Matorova) sites, respectively. Similarly, the corresponding yearly average concentrations of EC ranged between 0.095-0.48, 0.090-0.2 and 0.010-0.086 & mu;g m 3 at those sites. A clear seasonal variation in OC and EC concentrations was observed at each measurement site. OC concentrations were highest during summertime whereas EC concentrations were highest in wintertime. The seasonality of OC was clearest at the Arctic site that had also the largest temperature variation and shortest growing season resulting in a sharp increase in OC concentrations from June to August. At all the measurement sites, OC concentrations gradually increased when the temperature rose over sub-zero temperatures whereas the daily average EC concentrations did not show as apparent temperature dependence as OC. Based on the cluster analysis, highest OC and EC concentrations, and the highest total load for EC (23-32%), at all the sites were detected with the air mass origin of southeast. In the marine environment, the effect of black carbon from ship plumes was investigated. The limit for ship fuel sulfur content changed during the measurement period (in January 2015), but it was not observed to influence the Optical EC concentrations. Overall, long-term, continuous measurements are crucial when the time trends in air quality and the effect of emission mitigation actions are investigated. In this study, a slight decrease in OC was observed at the Marine site, however, a decrease for EC was seen both at the rural and marine sites suggesting that the emission mitigation actions like EURO limits for light vehicles or improved after-treatment systems developed for industry and energy production have already decreased the background concentrations in rural areas.
Recent recommendations given by WHO include systematic measurements of ambient particle number concentration and black carbon (BC) concentrations. In India and several other highly polluted areas, the air quality problems are severe and the need for air quality related information is urgent. This study focuses on particle number emissions and BC emissions of passenger cars that are technologically relevant from an Indian perspective. Particle number and BC were investigated under real-world conditions for driving cycles typical for Indian urban environments. Two mobile laboratories and advanced aerosol and trace gas instrumentation were utilized. Our study shows that passenger cars without exhaust particle filtration can emit in real-world conditions large number of particles, and especially at deceleration a significant fraction of particle number can be even in 1.5-10 nm particle sizes. The mass concentration of exhaust plume particles was dominated by BC that was emitted especially at acceleration conditions. However, exhaust particles contained also organic compounds, indicating the roles of engine oil and fuel in exhaust particle formation. In general, our study was motivated by serious Indian air quality problems, by the recognized lack of emission information related to Indian traffic, and by the recent WHO air quality guidance; our results emphasize the importance of monitoring particle number concentrations and BC also in Indian urban areas and especially in traffic environments where people can be significantly exposed to fresh exhaust emissions.
Ambient particles from natural and anthropogenic sources are a major cause of premature deaths globally. While there are many instruments suitable for scientific measurements of aerosols, better methods for long-term monitoring purposes are still needed, especially low-maintenance, affordable solutions for ultrafine particles. In this article, we present a new sensor design and prototype, the inherently charged particle (ICP) sensor, which uses the preexisting electrical charge of particles to measure particle concentration, instead of employing a charging mechanism, as is typical for instruments based on electrical detection. When the ICP-sensor is employed in conjunction with another instrument, information on the particle charge state can also be derived. We present the results of a laboratory characterization as well as two measurements in suggested applications: 1) engine exhaust measurements and 2) ambient measurements in a traffic environment, where we compare the sensor response to three particle concentration metrics: 1) number; 2) surface area; and 3) mass. The sensor proved suitable for both applications, the signal correlated best with number concentration in the engine emission measurements and with particle surface area in the ambient measurements. The measured charge concentrations were well-correlated ( ${R}^{\,2} >0.8$ ) with theoretical values calculated from the number size distribution assuming an equilibrium charge distribution.