Erkka Saukko

On-Line Characterization of Morphology and Water Adsorption on Fumed Silica Nanoparticles

The first wetting layer on solid nanoparticles has direct implications on the roles these particles play in industrial processes and technological applications as well as in the atmosphere. We present a technique for online measurements of the adsorption of the first few water layers onto insoluble aerosol nanoparticles. Atomized fumed silica nanoparticles were dispersed from aqueous suspension and their hygroscopic growth factors (HGF) and number of the adsorbed water layers at subsaturated conditions were measured using a nanometer hygroscopic tandem differential mobility analyzer (HTDMA). Particle morphology was characterized by electron microscopy and particle density was determined by mobility analysis. The HGFs of the size-selected particles at mobility diameters from 10 to 50 nm at 90% relative humidity (RH) varied from 1.05 to 1.24, corresponding to 2–6 layers of adsorbed water. The morphology of the generated fumed silica nanoparticles varied from spheres at 8–10 nm to agglomerates at larger diameters with effective density from 1.7 to 0.8 g/cm3 and fractal dimension of 2.6. The smallest spheres and agglomerates had the highest HGFs. The smallest particles with diameters of 8 and 10 nm adsorbed two to three water layers in subsaturated conditions, which agreed well with the Frenkel, Halsey, and Hill (FHH) isotherm fitting. In comparison to the small spheres or large agglomerates, the compact agglomerate structure containing a few primary particles increased the number of adsorbed water layers by a factor of ∼1.5. This was probably caused by the capillary effect on the small cavities between the primary particles in the agglomerate.

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.

Phase state and deliquescence hysteresis of ammonium sulfate seeded secondary organic aerosol

The phase state of secondary organic aerosol (SOA) has an impact on its lifetime, composition, and its interaction with water. To better understand the effect of phase state of SOA on climate interactions, we studied the SOA phase state and the effect of its history and report here the phase state and the humidity-induced phase hysteresis of multicomponent-seeded SOA particles produced in a large, continuously stirred tank reactor. We determined the phase state of the particles by their bounced fraction impacting on a smooth substrate in a low-pressure impactor. The particles were composed of ammonium sulfate ([NH4]2SO4) seed and a secondary organic matter (SOM) shell formed from oxidized α-pinene or isoprene. The ammonium sulfate (AS) seed dominated the deliquescence of the α-pinene SOM multicomponent particles, whereas their efflorescence was strongly attenuated by the SOM coating. Particles coated with isoprene SOM showed continuous phase transitions with a lesser effect by the AS seed. The results agree with and independently corroborate contemporary research. Copyright 2015 American Association for Aerosol Research

Ion Mobility Distributions during the Initial Stages of New Particle Formation by the Ozonolysis of α-Pinene

An ion mobility spectrometer (IMS) was used to study gas phase compounds during nucleation and growth of secondary organic aerosols (SOA). In this study SOA particles were generated by oxidizing α-pinene with O(3) and OH in a 6 m(3) reaction chamber. Positive ion peaks with reduced mobilities of 1.59 cm(2)(Vs)(-1) and 1.05 cm(2)(Vs)(-1) were observed 7 min after α-pinene and ozone were added to the chamber. The detected compounds can be associated with low volatility oxidation products of α-pinene, which have been suggested to participate in new particle formation. This is the first time that IMS has been applied to laboratory studies of SOA formation. IMS was found suitable for continuous online monitoring of the SOA formation process, allowing for highly sensitive detection of gas phase species that are thought to initiate new particle formation.

Characteristics of particle emissions and their atmospheric dilution during co-combustion of coal and wood pellets in a large combined heat and power plant

Abstract Coal combustion is one of the most significant anthropogenic CO2 and air pollution sources globally. This paper studies the atmospheric emissions of a power plant fuelled with a mixture of industrial pellets (10.5%) and coal (89.5%). Based on the stack measurements, the solid particle number emission, which was dominated by sub-200 nm particles, was 3.4×1011 MJ-1 for the fuel mixture when electrostatic precipitator (ESP) was cleaning the flue gas. The emission factor was 50 mg MJ-1 for particulate mass and 11 740 ng MJ-1 for the black carbon with the ESP. In the normal operation situation of the power plant, i.e., including the flue-gas desulphurisation and fabric filters (FGD and FF), the particle number emission factor was 1.7×108 MJ-1, particulate mass emission factor 2 mg MJ-1 and black carbon emission factor 14 ng MJ-1. Transmission electron microscopy (TEM) analysis supported the particle number size distribution measurement in terms of particle size and the black carbon concentration. The TEM images of the particles showed variability of the particle sizes, morphologies and chemical compositions. The atmospheric measurements, conducted in the flue-gas plume, showed that the flue-gas dilutes closed to background concentrations in 200 sec. However, an increase in particle number concentration was observed when the flue gas aged. This increase in particle number concentration was interpret as formation of new particles in the atmosphere. In general, the study highlights the importance of detailed particle measurements when utilizing new fuels in existing power plants. Implications: CO2 emissions of energy production decrease when substituting coal with biofuels. The effects of fuels changes on particle emission characteristics have not been studied comprehensively. In this study conducted for a real-scale power plant, co-combustion of wood pellets and coal caused elevated black carbon emissions. However, it was beneficial from the total particle number and particulate mass emission point of view. Flue-gas cleaning can significantly decrease the pollutant concentrations but also changes the characteristics of emitted particles. Atmospheric measurements implicated that the new particle formation in the atmospheric flue-gas plume should be taken into account when evaluating all effects of fuel changes.” Are implication statements part of the manuscript?

Comparative performance of a thermal denuder and a catalytic stripper in sampling laboratory and marine exhaust aerosols

ABSTRACT The performance of a thermal denuder (thermodenuder—TD) and a fresh catalytic stripper (CS) was assessed by sampling laboratory aerosol, produced by different combinations of sulfuric acid, octacosane, and soot particles, and marine exhaust aerosol produced by a medium-speed marine engine using high sulfur fuels. The intention was to study the efficiency in separating non-volatile particles. No particles could be detected downstream of either device when challenged with neat octacosane particles at high concentration. Both laboratory and marine exhaust aerosol measurements showed that sub-23 nm semi-volatile particles are formed downstream of the thermodenuder when upstream sulfuric acid approached 100 ppbv. Charge measurements revealed that these are formed by re-nucleation rather than incomplete evaporation of upstream aerosol. Sufficient dilution to control upstream sulfates concentration and moderate TD operation temperature (250°C) are both required to eliminate their formation. Use of the CS following an evaporation tube seemed to eliminate the risk for particle re-nucleation, even at a ten-fold higher concentration of semi-volatiles than in case of the TD. Particles detected downstream of the CS due to incomplete evaporation of sulfuric acid and octacosane aerosol, did not exceed 0.01% of upstream concentration. Despite the superior performance of CS in separating non-volatile particles, the TD may still be useful in cases where increased sensitivity over the traditional evaporation tube method is needed and where high sulfur exhaust concentration may fast deplete the catalytic stripper adsorption capacity. Copyright