Suppression of nucleation mode particles by biomass burning in an urban environment: a case study.

Measurements of concentrations and size distributions of particles 4.7 to 160 nm were taken using an SMPS during the bonfire and firework celebrations on Bonfire Night in Leeds, UK, 2006. These celebrations provided an opportunity to study size distributions in a unique atmospheric pollution situation during and following a significant emission event due to open biomass burning. A log-normal fitting program was used to determine the characteristics of the modal groups present within hourly averaged size distributions. Results from the modal fitting showed that on bonfire night the smallest nucleation mode, which was present before and after the bonfire event and on comparison weekends, was not detected within the size distribution. In addition, there was a significant shift in the modal diameters of the remaining modes during the peak of the pollution event. Using the concept of a coagulation sink, the atmospheric lifetimes of smaller particles were significantly reduced during the pollution event, and thus were used to explain the disappearance of the smallest nucleation mode as well as changes in particle count mean diameters. The significance for particle mixing state is discussed.

Factors influencing particle number concentrations, size distributions and modal parameters at a roof-level and roadside site in Leicester, UK.

Measurements of urban particle number concentrations and size distributions in the range 5-1000 nm were taken at elevated (roof-level) and roadside sampling sites on Narborough Road in Leicester, UK, along with simultaneous measurements of traffic, NO(x), CO and 1,3-butadiene concentrations and meteorological parameters. A fitting program was used to determine the characteristics of up to five modal groups present in the particle size distributions. All particle modal concentrations peaked during the morning and evening rush hours. Additional events associated with the smallest mode, that were not observed to be connected to primary emissions, were also present suggesting that this mode consisted of newly formed secondary particles. These events included peaks in concentration which coincided with peaks in solar radiation, and lower concentrations of the larger modes. Investigation into the relationships between traffic flow and occupancy indicated three flow regimes; free-flow, unstable and congested. During free-flow conditions, positive linear relationships existed between traffic flow and particle modal number concentrations. However, during unstable and congested periods, this relationship was shown to break-down. Similar trends were observed for concentrations of the gas phase pollutants NO(x), CO and 1,3-butadiene. Strong linear relationships existed between NO(x), CO, 1,3-butadiene concentrations, nucleation and Aitken mode concentrations at both sampling locations, indicating a local traffic related emission source. At the roadside, both nucleation and Aitken mode are best represented by a decreasing exponential function with wind speed, whereas at the roof-level this relationship only occurred for Aitken mode particles. The differing relationships at the two sampling locations are most likely due to a combination of meteorological factors and distance from the local emission source.

The contributions to long-term health-relevant particulate matter at the UK EMEP supersites between 2010 and 2013: Quantifying the mitigation challenge.

Human health burdens associated with long-term exposure to particulate matter (PM) are substantial. The metrics currently recommended by the World Health Organization for quantification of long-term health-relevant PM are the annual average PM10 and PM2.5 mass concentrations, with no low concentration threshold. However, within an annual average, there is substantial variation in the composition of PM associated with different sources. To inform effective mitigation strategies, therefore, it is necessary to quantify the conditions that contribute to annual average PM10 and PM2.5 (rather than just short-term episodic concentrations). PM10, PM2.5, and speciated water-soluble inorganic, carbonaceous, heavy metal and polycyclic aromatic hydrocarbon components are concurrently measured at the two UK European Monitoring and Evaluation Programme (EMEP) 'supersites' at Harwell (SE England) and Auchencorth Moss (SE Scotland). In this work, statistical analyses of these measurements are integrated with air-mass back trajectory data to characterise the 'chemical climate' associated with the long-term health-relevant PM metrics at these sites. Specifically, the contributions from different PM concentrations, months, components and geographic regions are detailed. The analyses at these sites provide policy-relevant conclusions on mitigation of (i) long-term health-relevant PM in the spatial domain for which these sites are representative, and (ii) the contribution of regional background PM to long-term health-relevant PM. At Harwell the mean (±1 sd) 2010-2013 annual average concentrations were PM10=16.4±1.4µgm(-3) and PM2.5=11.9±1.1µgm(-3) and at Auchencorth PM10=7.4±0.4µgm(-3) and PM2.5=4.1±0.2µgm(-3). The chemical climate state at each site showed that frequent, moderate hourly PM10 and PM2.5 concentrations (defined as approximately 5-15µgm(-3) for PM10 and PM2.5 at Harwell and 5-10µgm(-3) for PM10 at Auchencorth) determined the magnitude of annual average PM10 and PM2.5 to a greater extent than the relatively infrequent high, episodic PM10 and PM2.5 concentrations. These moderate PM10 and PM2.5 concentrations were derived across the range of chemical components, seasons and air-mass pathways, in contrast to the highest PM concentrations which tended to associate with specific conditions. For example, the largest contribution to moderate PM10 and PM2.5 concentrations - the secondary inorganic aerosol components, specifically NO3(-) - were accumulated during the arrival of trajectories traversing the spectrum of marine, UK, and continental Europe areas. Mitigation of the long-term health-relevant PM impact in the regions characterised by these two sites requires multilateral action, across species (and hence source sectors), both nationally and internationally; there is no dominant determinant of the long-term PM metrics to target.

Genotoxicity of size-fractionated samples of urban particulate matter.

Urban particulate matter (UPM) includes particles of size smaller than 10 microm (PM10), which may impact on human respiratory and cardiovascular health. It has been reported previously that PM10 can induce DNA damage. We have collected size-fractionated PM10 at the roadside and measured the induction of DNA damage by different-sized UPM using the alkaline Comet assay and the plasmid strand-break assay. We found that foil disks were more suitable for collecting UPM than quartz fiber filters, as the UPM could be easily extracted from the foil disks and accurately weighed. Using the Comet assay, all size fractions induced DNA damage in A549 lung epithelial cells, with the finer fractions (D50% = 0.65 microm and lower) inducing the most damage. In the plasmid strand-break assay, in which DNA damage is induced by free-radical species generated in solution, the most damage was also induced by the finer fractions, although the finest fraction (D50% < 0.43 microm) did not induce as much damage as D50% = 0.65 and 0.43 microm. When an organic extract of a standard UPM sample was compared to the whole particles and the washed particles in the Comet assay, it was found that around 75% of the damage induced by the whole UPM could be induced by the organic extract. These results show that finer particulates have the greatest ability to induce DNA damage in lung epithelial cells and naked DNA, and that both organic and inorganic components of the UPM contribute to its genotoxic effects.

Observations of urban airborne particle number concentrations during rush-hour conditions: analysis of the number based size distributions and modal parameters.

A summertime study of the number concentration and the size distribution of combustion derived nanometre sized particles (termed nanoparticles) from diesel and spark-ignition (SI) engine emissions were made under rush-hour and free-flow traffic conditions at an urban roadside location in Leeds, UK in July 2003. The measured total particle number concentrations (N(TOTAL)) were of the order 1.8 x 10(4) to 3.4 x 10(4) cm(-3), and tended to follow the diurnal traffic flow patterns. The N(TOTAL) was dominated by particles < or =100 nm in diameter which accounted for between 89-93% of the measured particle number. By use of a log-normal fitting procedure, the modal parameters of the number based particle size distribution of urban airborne particulates were derived from the roadside measurements. Four component modes were identified. Two nucleation modes were found, with a smaller, more minor, mode composed principally of sub-11 nm particles, believed to be derived from particles formed from the nucleation of gaseous species in the atmosphere. A second mode, much larger in terms of number, was composed of particles within the size range of 10-20 nm. This second mode was believed to be principally derived from the condensation of the unburned fuel and lube oil (the solvent organic fraction or SOF) as it cooled on leaving the engine exhaust. Third and fourth modes were noted within the size ranges of 28-65 nm and 100-160 nm, respectively. The third mode was believed to be representative of internally mixed Aitken mode particles composed of a soot/ash core with an adsorbed layer of readily volatilisable material. The fourth mode was believed to be composed of chemically aged, secondary particles. The larger nucleation and Aitken modes accounted for between 80-90% of the measured N(TOTAL), and the particles in these modes were believed to be derived from SI and diesel engine emissions. The overall size distribution, particularly in modes II-IV, was observed to be strongly related to the number of primary particle emissions, with larger count median diameters observed under conditions where low numbers of primary soot based particles were present.