The characteristics of the nucleation mode particles of a Euro IV heavy-duty diesel vehicle exhaust were studied. The NOx and PM emissions of the vehicle were controlled through the use of cooled EGR and high-pressure fuel injection techniques; no exhaust gas after-treatment was used. Particle measurements were performed in vehicle laboratory and on road. Nucleation mode dominated the particle number size distribution in all the tested driving conditions. According to the on-road measurements, the nucleation mode was already formed after 0.7 s residence time in the atmosphere and no significant changes were observed for longer residence times. The nucleation mode was insensitive to the fuel sulfur content, dilution air temperature, and relative humidity. An increase in the dilution ratio decreased the size of the nucleation mode particles. This behavior was observed to be linked to the total hydrocarbon concentration in the diluted sample. In volatility measurements, the nucleation mode particles were observed to have a nonvolatile core with volatile species condensed on it. The results indicate that the nucleation mode particles have a nonvolatile core formed before the dilution process. The core particles have grown because of the condensation of semivolatile material, mainly hydrocarbons, during the dilution.

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 2.4·10 15 (kg fuel ) −1 in a roadside environment, 2.6·10 15 (kg fuel ) −1 in a street canyon, and 2.9·10 15 (kg fuel ) −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 1.6·10 12 (kg fuel ) −1 to a high value of 4.3·10 15 (kg fuel ) −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.nanocluster aerosol | atmospheric aerosol | combustion-derived nanoparticles | air pollution | traffic emission D etailed characterization of aerosol sources is required to understand climate impacts and health effects of atmospheric aerosols, as well as to develop technologies and policies capable of mitigating air pollution in urbanized areas. In densely populated areas, one of the most significant source of particles is traffic (1, 2). Owing to their small size and complicated chemical and physical characteristics (3-6), atmospheric particles resulting from traffic emissions pose a significant risk to human health (7-12), and also contribute to anthropogenic forcing of climate (13,14). Previous research on vehicular emissions has demonstrated the presence of soot and ash (3, 15) and solid sub-10-nm core particles (4-6) in primary emissions from vehicles and engines and their variation, depending on vehicle technologies (4, 6), the properties of fuels and lubricant oils (15, 16), and driving conditions (15-17). In addition to particles, exhaust typically contains species that reside in the gaseous phase in the undiluted high-temperature exhaust (5, 18, 19) but condense or even nucleate to the particle phase immediately after the exhaust is released to the atmosphere. Here, we term such aerosols delayed primary aerosols, because particle precursors exist already in the u...

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To mitigate the diesel particle pollution problem, diesel vehicles are fitted with modern exhaust after-treatment systems (ATS), which efficiently remove engine-generated primary particles (soot and ash) and gaseous hydrocarbons. Unfortunately, ATS can promote formation of low-vapor-pressure gases, which may undergo nucleation and condensation leading to formation of nucleation particles (NUP). The chemical nature and formation mechanism of these particles are only poorly explored. Using a novel mass spectrometric method, online measurements of low-vapor-pressure gases were performed for exhaust of a modern heavy-duty diesel engine operated with modern ATS and combusting low and ultralow sulfur fuels and also biofuel. It was observed that the gaseous sulfuric acid (GSA) concentration varied strongly, although engine operation was stable. However, the exhaust GSA was observed to be affected by fuel sulfur level, exhaust after-treatment, and driving conditions. Significant GSA concentrations were measured also when biofuel was used, indicating that GSA can be originated also from lubricant oil sulfur. Furthermore, accompanying NUP measurements and NUP model simulations were performed. We found that the exhaust GSA promotes NUP formation, but also organic (acidic) precursor gases can have a role. The model results indicate that that the measured GSA concentration alone is not high enough to grow the particles to the detected sizes.

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Abstract. Four measurement campaigns were performed in two different environments -inside the harbour areas in the city centre of Helsinki, and along the narrow shipping channel near the city of Turku, Finland -using a mobile laboratory van during winter and summer conditions in 2010-2011. The characteristics of gaseous (CO, CO 2 , SO 2 , NO, NO 2 , NO x ) and particulate (number and volume size distributions as well as PM 2.5 ) emissions for 11 ships regularly operating on the Baltic Sea were studied to determine the emission parameters. The highest particle concentrations were 1.5 × 10 6 and 1.6 × 10 5 cm −3 in Helsinki and Turku, respectively, and the particle number size distributions had two modes. The dominating mode peaked at 20-30 nm, and the accumulation mode at 80-100 nm. The majority of the particle mass was volatile, since after heating the sample to 265 • C, the particle volume of the studied ship decreased by around 70 %. The emission factors for NO x varied in the range of 25-100 g (kg fuel) −1 , for SO 2 in the range of 2.5-17.0 g (kg fuel) −1 , for particle number in the range of (0.32-2.26) × 10 16 # (kg fuel) −1 , and for PM 2.5 between 1.0-4.9 g (kg fuel) −1 . The ships equipped with SCR (selective catalytic reduction) had the lowest NO x emissions, whereas the ships with DWI (direct water injection) and HAMs (humid air motors) had the lowest SO 2 emissions but the highest particulate emissions. For all ships, the averaged fuel sulphur contents (FSCs) were less than 1 % (by mass) but none of them was below 0.1 % which will be the new EU directive starting 1 January 2015 in the SO x emission control areas; this indicates that ships operating on the Baltic Sea will face large challenges.

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