Hilkka Timonen

Chemical composition of fine particles in fresh smoke plumes from boreal wild-land fires in Europe.

A series of smoke plumes was detected in Helsinki, Finland, during a one-month-lasting period in August 2006. The smoke plumes originated from wildfires close to Finland, and they were short-term and had a high particulate matter (PM) concentration. Physical and chemical properties of fine particles in those smokes were characterised by a wide range of real-time measurements that enabled the examination of individual plume events. Concurrently PM(1) filter samples were collected and analysed off-line. Satellite observations employing MODIS sensor on board of NASA EOS Terra satellite with the dispersion model SILAM and the Fire Assimilation System were used for evaluation of the emission fluxes from wildfires. The model predicted well the timing of the plumes but the predicted PM concentrations differed from the observed. The measurements showed that the major growth in PM concentration was caused by submicrometer particles consisting mainly of particulate organic matter (POM). POM had not totally oxidised during the transport based on the low WSOC-to-OC ratio. The fresh plumes were compared to another major smoke episode that was observed in Helsinki during April-May 2006. The duration and the source areas of the two episode periods differed. The episode in April-May was a period of nearly constantly upraised level of long-range transported PM and it was composed of aged particles when arriving in Helsinki. The two episodes had differences also in the chemical composition of PM. The mass concentrations of biomass burning tracers (levoglucosan, potassium, and oxalate) increased during both the episodes but different concentration levels of elemental carbon and potassium indicated that the episodes differed in the form of burning as well as in the burning material. In spring dry crop residue and hay from the previous season were burnt whereas in August smokes from smouldering and incomplete burning of fresh vegetation were detected.

BAECC: A Field Campaign to Elucidate the Impact of Biogenic Aerosols on Clouds and Climate

AbstractDuring Biogenic Aerosols—Effects on Clouds and Climate (BAECC), the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program deployed the Second ARM Mobile Facility (AMF2) to Hyytiala, Finland, for an 8-month intensive measurement campaign from February to September 2014. The primary research goal is to understand the role of biogenic aerosols in cloud formation. Hyytiala is host to the Station for Measuring Ecosystem–Atmosphere Relations II (SMEAR II), one of the world’s most comprehensive surface in situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions, and an extensive suite of parameters relevant to atmosphere–biosphere interactions continuously since 1996. Combining vertical profiles from AMF2 with surface-based in situ SMEAR II observations allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. Together with the inclusion of extensi...

Physical and Chemical Characterization of Real-World Particle Number and Mass Emissions from City Buses in Finland.

Exhaust emissions of 23 individual city buses at Euro III, Euro IV and EEV (Enhanced Environmentally Friendly Vehicle) emission levels were measured by the chasing method under real-world conditions at a depot area and on the normal route of bus line 24 in Helsinki. The buses represented different technologies from the viewpoint of engines, exhaust after-treatment systems (ATS) and fuels. Some of the EEV buses were fueled by diesel, diesel-electric, ethanol (RED95) and compressed natural gas (CNG). At the depot area the emission factors were in the range of 0.3-21 × 10(14) # (kg fuel)(-1), 6-40 g (kg fuel)(-1), 0.004-0.88 g (kg fuel)(-1), 0.004-0.56 g (kg fuel)(-1), 0.01-1.2 g (kg fuel)(-1), for particle number (EFN), nitrogen oxides (EFNOx), black carbon (EFBC), organics (EFOrg), and particle mass (EFPM1), respectively. The highest particulate emissions were observed from the Euro III and Euro IV buses and the lowest from the ethanol and CNG-fueled buses, which emitted BC only during acceleration. The organics emitted from the CNG-fueled buses were clearly less oxidized compared to the other bus types. The bus line experiments showed that lowest emissions were obtained from the ethanol-fueled buses whereas large variation existed between individual buses of the same type indicating that the operating conditions by drivers had large effect on the emissions.

Wintertime Aerosol Chemistry in Sub-Arctic Urban Air

Measurements of submicron particulate matter (PM) were performed at an urban background station, in Helsinki, Finland during wintertime to investigate the chemical characteristics and sources of PM1. The PM1 was dominated by sulfate and organics. The source apportionment indicated that organic aerosol (OA) was a mixture from local sources (biomass burning (BBOA), traffic, coffee roaster (CROA)), secondary compounds formed in local wintertime conditions (nitrogen containing OA (NOA), semivolatile oxygenated OA (SV-OOA), and regional and long-range transported compounds (low volatile oxygenated OA, LV-OOA). BBOA was dominated by the fragments C2H4O2 + and C3H4O2 + (m/z 60.021 and 73.029) from levoglucosan, or other similar sugar components, comprising on average 32% of the BBOA mass concentration. The ratio between fragments C2H4O2 +/C3H4O2 + was significantly lower for CROA (=1.1) when compared to BBOA (=2.1), indicating that they consisted of different sugar compounds. In addition, a component containing substantial amount of nitrogen compounds (NOA) was observed in a sub-arctic region for the first time. The NOA contribution to OA ranged from 1% to 29% and elevated concentrations were observed when ambient relative humidity was high and the visibility low. Low solar radiation and temperature in wintertime were observed to influence the oxidation of compounds. A change in aerosol composition, with an increase of LV-OOA and decrease in BBOA, SV-OOA and NOA was noticed during the transition from wintertime to springtime. Size distribution measurements with high-time resolution enabled chemical characterization of externally mixed aerosol from different sources. Aged regional long-range transported aerosols were dominant at around 0.5 μm (vacuum aerodynamic diameter), whereas traffic and CROA emissions dominated at around 120 nm. Copyright 2014 American Association for Aerosol Research

Traffic is a major source of atmospheric nanocluster aerosol

Significance We report the significant presence of traffic-originated nanocluster aerosol (NCA) particles in a particle diameter range of 1.3–3.0 nm of urban air, determine the emission factors for the NCA, and evaluate its global importance. Our findings are important because they significantly update the current understanding of atmospheric aerosol in urban areas. They demonstrate that in urban air, extremely small particles form a significant fraction of the total particle number and are a direct result of anthropogenic emissions, that is, the emissions from road traffic. Thus, our findings also imply that in urban areas, an atmospheric nucleation process is not necessary for the formation of a large number of particles that affect population health and climate. In densely populated areas, traffic is a significant source of atmospheric aerosol particles. Owing to their small size and complicated chemical and physical characteristics, atmospheric particles resulting from traffic emissions pose a significant risk to human health and also contribute to anthropogenic forcing of climate. Previous research has established that vehicles directly emit primary aerosol particles and also contribute to secondary aerosol particle formation by emitting aerosol precursors. Here, we extend the urban atmospheric aerosol characterization to cover nanocluster aerosol (NCA) particles and show that a major fraction of particles emitted by road transportation are in a previously unmeasured size range of 1.3–3.0 nm. For instance, in a semiurban roadside environment, the NCA represented 20–54% of the total particle concentration in ambient air. The observed NCA concentrations varied significantly depending on the traffic rate and wind direction. The emission factors of NCA for traffic were 2.4·1015 (kgfuel)−1 in a roadside environment, 2.6·1015 (kgfuel)−1 in a street canyon, and 2.9·1015 (kgfuel)−1 in an on-road study throughout Europe. Interestingly, these emissions were not associated with all vehicles. In engine laboratory experiments, the emission factor of exhaust NCA varied from a relatively low value of 1.6·1012 (kgfuel)−1 to a high value of 4.3·1015 (kgfuel)−1. These NCA emissions directly affect particle concentrations and human exposure to nanosized aerosol in urban areas, and potentially may act as nanosized condensation nuclei for the condensation of atmospheric low-volatile organic compounds.

Natural Gas Engine Emission Reduction by Catalysts

In order to meet stringent emission limits, after-treatment systems are increasingly utilized in natural gas engine applications. In this work, two catalyst systems were studied in order to clarify how the catalysts affect, e.g. hydrocarbons, NOx and particles present in natural gas engine exhaust. A passenger car engine modified to run with natural gas was used in a research facility with possibilities to modify the exhaust gas properties. High NOx reductions were observed when using selective catalytic reduction, although a clear decrease in the NOx reduction was recorded at higher temperatures. The relatively fresh methane oxidation catalyst was found to reach reductions greater than 50% when the exhaust temperature and the catalyst size were sufficient. Both the studied catalyst systems were found to have a significant effect on particulate emissions. The observed particle mass reduction was found to be due to a decrease in the amount of organics passing over the catalyst. However, especially at high exhaust temperatures, high nanoparticle concentrations were observed downstream of the catalysts together with higher sulphate concentrations in particles. This study contributes to understanding emissions from future natural gas engine applications with catalysts in use.

Investigating the chemical species in submicron particles emitted by city buses

ABSTRACT Detailed chemical characterization of exhaust particles from 23 individual city buses was performed in Helsinki, Finland. Investigated buses represented different technologies in terms of engines, exhaust after-treatment systems (e.g., diesel particulate filter, selective catalytic reduction, and three-way catalyst) and fuels (diesel, diesel-electric (hybrid), ethanol, and compressed natural gas). Regarding emission standards, the buses operated at EURO III, EURO IV, and EEV (enhanced environmentally friendly vehicle) emission levels. The chemical composition of exhaust particles was determined by using a soot particle aerosol mass spectrometer (SP-AMS). Based on the SP-AMS results, the bus emission particles were dominated by organics and refractory black carbon (rBC). The mass spectra of organics consisted mostly of hydrocarbon fragments (54–86% of total organics), the pattern of hydrocarbon fragments being rather similar regardless of the bus type. Regarding oxygenated organic fragments, ethanol-fueled buses had unique mass-to-charge ratios (m/z) of 45, 73, 87, and 89 (mass fragments of C2H5O+, C3H5O2+, C4H7O2+, and C4H9O2+, respectively) that were not detected for the other bus types at the same level. For rBC, there was a small difference in the ratio of C4+ and C5+ to C3+ for different bus types but also for the individual buses of the same type. In addition to organics and rBC, the presence of trace metals in the bus emission particles was investigated. Copyright

Response Characterization of an Inexpensive Aerosol Sensor

Inexpensive aerosol sensors have been considered as a complementary option to address the issue of expensive but low spatial coverage air quality monitoring networks. However, the accuracy and response characteristics of these sensors is poorly documented. In this study, inexpensive Shinyei PPD42NS and PPD60PV sensors were evaluated using a novel laboratory evaluation method. A continuously changing monodisperse size distribution of particles was generated using a Vibrating Orifice Aerosol Generator. Furthermore, the laboratory results were validated in a field experiment. The laboratory tests showed that both of the sensors responded to particulate mass (PM) concentration stimulus, rather than number concentration. The highest detection efficiency for the PPD42NS was within particle size range of 2.5–4 µm, and the respective optimal size range for the PPD60PV was 0.7–1 µm. The field test yielded high PM correlations (R2 = 0.962 and R2 = 0.986) for viable detection ranges of 1.6–5 and 0.3–1.6 µm, when compared to a medium cost optical dust monitor. As the size distribution of atmospheric particles tends to be bimodal, it is likely that indicatively valid results could be obtained for the PM10–2.5 size fraction (particulate mass in size range 2.5–10 µm) with the PPD42NS sensor. Respectively, the PPD60PV could possibly be used to measure the PM2.5 size fraction (particulate mass in size below 2.5 µm).

Spatiotemporal Variation in Composition of Submicron Particles in Santiago Metropolitan Region, Chile

The chemical composition of submicron particles (aerodynamic diameter Da < 1.0 μm) was investigated at three locations in the Santiago Metropolitan Region (SMR), Chile. Measurements campaigns were conducted in winter and spring 2016, at representative sites of a rural, urban and urban receptor environment. Instrumentation consisted of an optical analyzer to determine Black Carbon (BC) and the Aerosol Chemical Speciation Monitor (ACSM) to measure concentrations of particulate chloride (Cl-), nitrate (NO3-), sulfate (SO42-), ammonium (NH4+) and non-refractory carbonaceous species (organics). Complementary data, such as ozone concentration and meteorological parameters were obtained from the public air quality network. Results showed that in both the winter and spring seasons the organics predominated in the mass of submicron particles. This fraction was followed in decreasing order by NO3-, NH4+, BC, SO42- and Cl-. The highest average organics concentrations were measured in winter at the urban (32.2 µg m–3) and urban receptor sites (20.1 µg m–3). In winter, average concentrations of both NO3- and NH4+ were higher at the urban receptor site (12.3 and 4.5 µg m–3, respectively) when compared to the urban site (6.4 and 3.1 µg m–3, respectively). In general, all the measured species were present in higher concentrations during winter, excepting SO42-, which was the only one that increased during spring. The transition towards spring was also associated with an acidification of the aerosol at the rural and urban receptor site, while at the urban site the aerosol was observed alkaline. The highest average ozone concentration during both the winter and spring seasons were recorded at the urban receptor site (7.2 and 24.0 ppb, respectively). The study reports data showing that the atmosphere in the SRM has a considerable load of particulate organic compounds, NO3- and NH4+, which are in higher concentrations at urban sites during the winter season. Based on wind patterns and the hourly profiles of chemical species, the study suggests that during daytime the polluted air masses from the urban center can move to the northeast part of the region (namely urban receptor site) leading to the formation of submicron particles as well as photochemical ozone.

Vertical profiles of lung deposited surface area concentration of particulate matter measured with a drone in a street canyon

The vertical profiles of lung deposited surface area (LDSA) concentration were measured in an urban street canyon in Helsinki, Finland, by using an unmanned aerial system (UAS) as a moving measurement platform. The street canyon can be classified as an avenue canyon with an aspect ratio of 0.45 and the UAS was a multirotor drone especially modified for emission measurements. In the experiments of this study, the drone was equipped with a small diffusion charge sensor capable of measuring the alveolar LDSA concentration of particles. The drone measurements were conducted during two days on the same spatial location at the kerbside of the street canyon by flying vertically from the ground level up to an altitude of 50 m clearly above the rooftop level (19 m) of the nearest buildings. The drone data were supported by simultaneous measurements and by a two-week period of measurements at nearby locations with various instruments. The results showed that the averaged LDSA concentrations decreased approximately from 60 μm2/cm3 measured close to the ground level to 36-40 μm2/cm3 measured close to the rooftop level of the street canyon, and further to 16-26 μm2/cm3 measured at 50 m. The high-resolution measurement data enabled an accurate analysis of the functional form of vertical profiles both in the street canyon and above the rooftop level. In both of these regions, exponential fits were used and the parameters obtained from the fits were thoroughly compared to the values found in literature. The results of this study indicated that the role of turbulent mixing caused by traffic was emphasized compared to the street canyon vortex as a driving force of the dispersion. In addition, the vertical profiles above the rooftop level showed a similar exponential decay compared to the profiles measured inside the street canyon.