974 resultados para sekundäres organisches Aerosol


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As part of a larger indoor environmental study, residential indoor and outdoor levels of nitrogen dioxide (NO2) were measured for 14 houses in a suburb of Brisbane, Queensland, Australia. Passive samplers were used for 48-h sampling periods during the winter of 1999. The average indoor and outdoor NO2 levels were 13.8 ± 6.3 and 16.7 ± 4.2 ppb, respectively. The indoor/outdoor NO2 concentration ratio ranged from 0.4 to 2.3, with a median value of 0.82. The results of statistic analyses indicated that there was no significant correlation between indoor and outdoor NO2 concentrations, or between indoor and fixed site NO2 monitoring station concentrations. However, there was a significant correlation between outdoor and fixed site NO2 monitoring station concentrations. There was also a significant correlation between indoor NO2 concentration and indoor submicrometre (0.007–0.808 μm) aerosol particle number concentrations. The results in this study indicated indoor NO2 levels are significantly affected by indoor NO2 sources, such as a gas stove and cigarette smoking. It implies that the outdoor or fixed site monitoring concentration alone is a poor predictor of indoor NO2 concentration.

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Dry powder inhaler (DPI) formulations is one of the most useful aerosol preparations in which drugs may be formulated as carrier-based interactive mixtures with micronised drug particles (<5 μm) adhered onto the surface of large inert carriers (lactose powders). The addition of magnesium stearate (MgSt) (1-3), was found to increase dispersion of various drugs from DPI formulations. Recently, some active compounds coated with 5% (wt/wt) MgSt using the mechanofusion method showed significant improvements in aerosolization behavior due to the reduction in intrinsic cohesion force (4). Application of MgSt in powder formulations is not new; however, no studies demonstrated the minimum threshold level for this excipient in efficient aerosolization of drug powders from the interactive mixtures. Therefore, this study investigated the role of MgSt concentration on the efficient dispersion of salbutamol sulphate (SS) from DPI formulations.

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The role of ions in the production of atmospheric particles has gained wide interest due to their profound impact on climate. Away from anthropogenic sources, molecules are ionized by alpha radiation from radon exhaled from the ground and cosmic gamma radiation from space. These molecular ions quickly form into ‘cluster ions’, typically smaller than about 1.5 nm. Using our measurements and the published literature, we present evidence to show that cluster ion concentrations in forest areas are consistently higher than outside. Since alpha radiation cannot penetrate more than a few centimetres of soil, radon present deep in the ground cannot directly contribute to the measured cluster ion concentrations. We propose an additional mechanism whereby radon, which is water soluble, is brought up by trees and plants through the uptake of groundwater and released into the atmosphere by transpiration. We estimate that, in a forest comprising eucalyptus trees spaced 4m apart, approximately 28% of the radon in the air may be released by transpiration. Considering that 24% of the earth’s land area is still covered in forests; these findings have potentially important implications for atmospheric aerosol formation and climate.

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Influenza is a widespread disease occurring in seasonal epidemics, and each year is responsible for up to 500,000 deaths worldwide. Influenza can develop into strains which cause severe symptoms and high mortality rates, and could potentially reach pandemic status if the virus’ properties allow easy transmission. Influenza is transmissible via contact with the virus, either directly (infected people) or indirectly (contaminated objects); via reception of large droplets over short distances (one metre or less); or through inhalation of aerosols containing the virus expelled by infected individuals during respiratory activities, that can remain suspended in the air and travel distances of more than one metre (the aerosol route). Aerosol transmission of viruses involves three stages: production of the droplets containing viruses; transport of the droplets and ability of a virus to remain intact and infectious; and reception of the droplets (via inhalation). Our understanding of the transmission of influenza viruses via the aerosol route is poor, and thus our ability to prevent a widespread outbreak is limited. This study explored the fate of viruses in droplets by investigating the effects of some physical factors on the recovery of both a bacteriophage model and influenza virus. Experiments simulating respiratory droplets were carried out using different types of droplets, generated from a commonly used water-like matrix, and also from an ‘artificial mucous’ matrix which was used to more closely resemble respiratory fluids. To detect viruses in droplets, we used the traditional plaque assay techniques, and also a sensitive, quantitative PCR assay specifically developed for this study. Our results showed that the artificial mucous suspension enhanced the recovery of infectious bacteriophage. We were able to report detection limits of infectious bacteriophage (no bacteriophage was detected by the plaque assay when aerosolised from a suspension of 103 PFU/mL, for three of the four droplet types tested), and that bacteriophage could remain infectious in suspended droplets for up to 20 minutes. We also showed that the nested real-time PCR assay was able to detect the presence of bacteriophage RNA where the plaque assay could not detect any intact particles. Finally, when applying knowledge from the bacteriophage experiments, we reported the quantitative recoveries of influenza viruses in droplets, which were more consistent and stable than we had anticipated. Influenza viruses can be detected up to 20 minutes (after aerosolisation) in suspended aerosols and possibly beyond. It also was detectable from nebulising suspensions with relatively low concentrations of viruses.

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Water uptake refers to the ability of atmospheric particles to take up water vapour from the surrounding atmosphere. This is an important property that affects particle size and phase and therefore influences many characteristics of aerosols relevant to air quality and climate. However, the water uptake properties of many important atmospheric aerosol systems, including those related to the oceans, are still not fully understood. Therefore, the primary aim of this PhD research program was to investigate the water uptake properties of marine aerosols. In particular, the effect of organics on marine aerosol water uptake was investigated. Field campaigns were conducted at remote coastal sites on the east coast of Australia (Agnes Water; March-April 2007) and west coast of Ireland (Mace Head; June 2007), and laboratory measurements were performed on bubble-generated sea spray aerosols. A combined Volatility-Hygroscopicity-Tandem Differential Mobility Analyser (VH-TDMA) was employed in all experiments. This system probes the changes in the hygroscopic properties of nanoparticles as volatile organic components are progressively evaporated. It also allows particle composition to be inferred from combined volatility-hygroscopicity measurements. Frequent new particle formation and growth events were observed during the Agnes Water campaign. The VH-TDMA was used to investigate freshly nucleated particles (17-22.5 nm) and it was found that the condensation of sulphate and/or organic vapours was responsible for driving particle growth during the events. Aitken mode particles (~40 nm) were also measured with the VH-TDMA. In 3 out of 18 VH-TDMA scans evaporation of a volatile, organic component caused a very large increase in hygroscopicity that could only be explained by an increase in the absolute water uptake of the particle residuals, and not merely an increase in their relative hygroscopicity. This indicated the presence of organic components that were suppressing the hygroscopic growth of mixed particles on the timescale of humidification in the VH-TDMA (6.5 secs). It was suggested that the suppression of water uptake was caused by either a reduced rate of hygroscopic growth due to the presence of organic films, or organic-inorganic interactions in solution droplets that had a negative effect on hygroscopicity. Mixed organic-inorganic particles were rarely observed by the VH-TDMA during the summer campaign conducted at Mace Head. The majority of particles below 100 nm in clean, marine air appeared to be sulphates neutralised to varying degrees by ammonia. On one unique day, 26 June 2007, particularly large concentrations of sulphate aerosol were observed and identified as volcanic emissions from Iceland. The degree of neutralisation of the sulphate aerosol by ammonia was calculated by the VH-TDMA and found to compare well with the same quantity measured by an aerosol mass spectrometer. This was an important verification of the VH-TMDA‘s ability to identify ammoniated sulphate aerosols based on the simultaneous measurement of aerosol volatility and hygroscopicity. A series of measurements were also conducted on sea spray aerosols generated from Moreton Bay seawater samples in a laboratory-based bubble chamber. Accumulation mode sea spray particles (38-173 nm) were found to contain only a minor organic fraction (< 10%) that had little effect on particle hygroscopicity. These results are important because previous studies have observed that accumulation mode sea spray particles are predominantly organic (~80% organic mass fraction). The work presented here suggests that this is not always the case, and that there may be currently unknown factors that are controlling the transfer of organics to the aerosol phase during the bubble bursting process. Taken together, the results of this research program have significantly improved our understanding of organic-containing marine aerosols and the way they interact with water vapour in the atmosphere.

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In recent years, the effect of ions and ultrafine particles on ambient air quality and human health has been well documented, however, knowledge about their sources, concentrations and interactions within different types of urban environments remains limited. This thesis presents the results of numerous field studies aimed at quantifying variations in ion concentration with distance from the source, as well as identifying the dynamics of the particle ionisation processes which lead to the formation of charged particles in the air. In order to select the most appropriate measurement instruments and locations for the studies, a literature review was also conducted on studies that reported ion and ultrafine particle emissions from different sources in a typical urban environment. The initial study involved laboratory experiments on the attachment of ions to aerosols, so as to gain a better understanding of the interaction between ions and particles. This study determined the efficiency of corona ions at charging and removing particles from the air, as a function of different particle number and ion concentrations. The results showed that particle number loss was directly proportional to particle charge concentration, and that higher small ion concentrations led to higher particle deposition rates in all size ranges investigated. Nanoparticles were also observed to decrease with increasing particle charge concentration, due to their higher Brownian mobility and subsequent attachment to charged particles. Given that corona discharge from high voltage powerlines is considered one of the major ion sources in urban areas, a detailed study was then conducted under three parallel overhead powerlines, with a steady wind blowing in a perpendicular direction to the lines. The results showed that large sections of the lines did not produce any corona at all, while strong positive emissions were observed from discrete components such as a particular set of spacers on one of the lines. Measurements were also conducted at eight upwind and downwind points perpendicular to the powerlines, spanning a total distance of about 160m. The maximum positive small and large ion concentrations, and DC electric field were observed at a point 20 m downwind from the lines, with median values of 4.4×103 cm-3, 1.3×103 cm-3 and 530 V m-1, respectively. It was estimated that, at this point, less than 7% of the total number of particles was charged. The electrical parameters decreased steadily with increasing downwind distance from the lines but remained significantly higher than background levels at the limit of the measurements. Moreover, vehicles are one of the most prevalent ion and particle emitting sources in urban environments, and therefore, experiments were also conducted behind a motor vehicle exhaust pipe and near busy motorways, with the aim of quantifying small ion and particle charge concentration, as well as their distribution as a function of distance from the source. The study found that approximately equal numbers of positive and negative ions were observed in the vehicle exhaust plume, as well as near motorways, of which heavy duty vehicles were believed to be the main contributor. In addition, cluster ion concentration was observed to decrease rapidly within the first 10-15 m from the road and ion-ion recombination and ion-aerosol attachment were the most likely cause of ion depletion, rather than dilution and turbulence related processes. In addition to the above-mentioned dominant ion sources, other sources also exist within urban environments where intensive human activities take place. In this part of the study, airborne concentrations of small ions, particles and net particle charge were measured at 32 different outdoor sites in and around Brisbane, Australia, which were classified into seven different groups as follows: park, woodland, city centre, residential, freeway, powerlines and power substation. Whilst the study confirmed that powerlines, power substations and freeways were the main ion sources in an urban environment, it also suggested that not all powerlines emitted ions, only those with discrete corona discharge points. In addition to the main ion sources, higher ion concentrations were also observed environments affected by vehicle traffic and human activities, such as the city centre and residential areas. A considerable number of ions were also observed in a woodland area and it is still unclear if they were emitted directly from the trees, or if they originated from some other local source. Overall, it was found that different types of environments had different types of ion sources, which could be classified as unipolar or bipolar particle sources, as well as ion sources that co-exist with particle sources. In general, fewer small ions were observed at sites with co-existing sources, however particle charge was often higher due to the effect of ion-particle attachment. In summary, this study quantified ion concentrations in typical urban environments, identified major charge sources in urban areas, and determined the spatial dispersion of ions as a function of distance from the source, as well as their controlling factors. The study also presented ion-aerosol attachment efficiencies under high ion concentration conditions, both in the laboratory and in real outdoor environments. The outcomes of these studies addressed the aims of this work and advanced understanding of the charge status of aerosols in the urban environment.

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Due to their large surface area, complex chemical composition and high alveolar deposition rate, ultrafine particles (UFPs) (< 0.1 ìm) pose a significant risk to human health and their toxicological effects have been acknowledged by the World Health Organisation. Since people spend most of their time indoors, there is a growing concern about the UFPs present in some indoor environments. Recent studies have shown that office machines, in particular laser printers, are a significant indoor source of UFPs. The majority of printer-generated UFPs are organic carbon and it is unlikely that these particles are emitted directly from the printer or its supplies (such as paper and toner powder). Thus, it was hypothesised that these UFPs are secondary organic aerosols (SOA). Considering the widespread use of printers and human exposure to these particles, understanding the processes involved in particle formation is of critical importance. However, few studies have investigated the nature (e.g. volatility, hygroscopicity, composition, size distribution and mixing state) and formation mechanisms of these particles. In order to address this gap in scientific knowledge, a comprehensive study including state-of-art instrumental methods was conducted to characterise the real-time emissions from modern commercial laser printers, including particles, volatile organic compounds (VOCs) and ozone (O3). The morphology, elemental composition, volatility and hygroscopicity of generated particles were also examined. The large set of experimental results was analysed and interpreted to provide insight into: (1) Emissions profiles of laser printers: The results showed that UFPs dominated the number concentrations of generated particles, with a quasi unimodal size distribution observed for all tests. These particles were volatile, non-hygroscopic and mixed both externally and internally. Particle microanalysis indicated that semi-volatile organic compounds occupied the dominant fraction of these particles, with only trace quantities of particles containing Ca and Fe. Furthermore, almost all laser printers tested in this study emitted measurable concentrations of VOCs and O3. A positive correlation between submicron particles and O3 concentrations, as well as a contrasting negative correlation between submicron particles and total VOC concentrations were observed during printing for all tests. These results proved that UFPs generated from laser printers are mainly SOAs. (2) Sources and precursors of generated particles: In order to identify the possible particle sources, particle formation potentials of both the printer components (e.g. fuser roller and lubricant oil) and supplies (e.g. paper and toner powder) were investigated using furnace tests. The VOCs emitted during the experiments were sampled and identified to provide information about particle precursors. The results suggested that all of the tested materials had the potential to generate particles upon heating. Nine unsaturated VOCs were identified from the emissions produced by paper and toner, which may contribute to the formation of UFPs through oxidation reactions with ozone. (3) Factors influencing the particle emission: The factors influencing particle emissions were also investigated by comparing two popular laser printers, one showing particle emissions three orders of magnitude higher than the other. The effects of toner coverage, printing history, type of paper and toner, and working temperature of the fuser roller on particle number emissions were examined. The results showed that the temperature of the fuser roller was a key factor driving the emission of particles. Based on the results for 30 different types of laser printers, a systematic positive correlation was observed between temperature and particle number emissions for printers that used the same heating technology and had a similar structure and fuser material. It was also found that temperature fluctuations were associated with intense bursts of particles and therefore, they may have impact on the particle emissions. Furthermore, the results indicated that the type of paper and toner powder contributed to particle emissions, while no apparent relationship was observed between toner coverage and levels of submicron particles. (4) Mechanisms of SOA formation, growth and ageing: The overall hypothesis that UFPs are formed by reactions with the VOCs and O3 emitted from laser printers was examined. The results proved this hypothesis and suggested that O3 may also play a role in particle ageing. In addition, knowledge about the mixing state of generated particles was utilised to explore the detailed processes of particle formation for different printing scenarios, including warm-up, normal printing, and printing without toner. The results indicated that polymerisation may have occurred on the surface of the generated particles to produce thermoplastic polymers, which may account for the expandable characteristics of some particles. Furthermore, toner and other particle residues on the idling belt from previous print jobs were a very clear contributing factor in the formation of laser printer-emitted particles. In summary, this study not only improves scientific understanding of the nature of printer-generated particles, but also provides significant insight into the formation and ageing mechanisms of SOAs in the indoor environment. The outcomes will also be beneficial to governments, industry and individuals.

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The deterioration of air quality is a significant issue in large and growing cities. This work investigates particulate emissions from transport, the largest source of air pollution in cities today. Emitters such as busy roads and diesel trains are investigated, with specific reference to the evolution of particles over time and distance. Diesel trains are investigated as an alternative to road traffic in investigating evolutionary processes. Higher emissions and solitary sources mean that the emitted plume can be observed over time in a single location. These results represent the first investigation of the evolution of fine and ultrafine aerosol particles from this type of source. Aerosols near a busy road are investigated, with the result that a dependence of total number concentration on distance from the road is shown to be related to the fragmentation of nanoparticle clusters. Local meteorological conditions are also monitored and humidity is shown to vary with distance from the road in a nonmonotonic way. Particles from a busy road were also examined using a scanning electron microscope, with the intention of understanding the make up of the emitted aerosol plume. It was determined that due to significant surface behaviour post-deposition, this method of analysis could not directly classify airborne pollutants. Some interesting results were obtained however, particularly in terms of composite particles and the analysis of deposited patterns. This thesis introduces new work in terms of the analysis of diesel train particulate emissions, as well as adding further evidence towards the fragmentation process of aerosol evolution in both background concentrations and emitted aerosol plumes.

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Positive and negative small ions, aerosol ion and number concentration and dc electric fields were monitored at an overhead high-voltage power line site. We show that the emission of corona ions was not spatially uniform along the lines and occurred from discrete components such as a particular set of spacers. Maximum ion concentrations and atmospheric dc electric fields were observed at a point 20 m downwind of the lines. It was estimated that less than 7% of the total number of aerosol particles was charged. The electrical parameters decreased steadily with further downwind distance but remained significantly higher than background.

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An increasing number of researchers have hypothesized that ozone may be involved in the particle formation processes that occur during printing, however no studies have investigated this further. In the current study, this hypothesis was tested in a chamber study by adding supplemental ozone to the chamber after a print job without measurable ozone emissions. Subsequent particle number concentration and size distribution measurements showed that new particles were formed minutes after the addition of ozone. The results demonstrated that ozone did react with printer-generated volatile organic compounds (VOCs) to form secondary organic aerosols (SOAs). The hypothesis was further confirmed by the observation of correlations among VOCs, ozone, and particles concentrations during a print job with measurable ozone emissions. The potential particle precursors were identified by a number of furnace tests, which suggested that squalene and styrene were the most likely SOA precursors with respect to ozone. Overall, this study significantly improved scientific understanding of the formation mechanisms of printer-generated particles, and highlighted the possible SOA formation potential of unsaturated nonterpene organic compounds by ozone-initiated reactions in the indoor environment. © 2011 American Chemical Society.

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Particles emitted by vehicles are known to cause detrimental health effects, with their size and oxidative potential among the main factors responsible. Therefore, understanding the relationship between traffic composition and both the physical characteristics and oxidative potential of particles is critical. To contribute to the limited knowledge base in this area, we investigated this relationship in a 4.5 km road tunnel in Brisbane, Australia. On-road concentrations of ultrafine particles (<100 nm, UFPs), fine particles (PM2.5), CO, CO2 and particle associated reactive oxygen species (ROS) were measured using vehicle-based mobile sampling. UFPs were measured using a condensation particle counter and PM2.5 with a DustTrak aerosol photometer. A new profluorescent nitroxide probe, BPEAnit, was used to determine ROS levels. Comparative measurements were also performed on an above-ground road to assess the role of emission dilution on the parameters measured. The profile of UFP and PM2.5 concentration with distance through the tunnel was determined, and demonstrated relationships with both road gradient and tunnel ventilation. ROS levels in the tunnel were found to be high compared to an open road with similar traffic characteristics, which was attributed to the substantial difference in estimated emission dilution ratios on the two roadways. Principal component analysis (PCA) revealed that the levels of pollutants and ROS were generally better correlated with total traffic count, rather than the traffic composition (i.e. diesel and gasoline-powered vehicles). A possible reason for the lack of correlation with HDV, which has previously been shown to be strongly associated with UFPs especially, was the low absolute numbers encountered during the sampling. This may have made their contribution to in-tunnel pollution largely indistinguishable from the total vehicle volume. For ROS, the stronger association observed with HDV and gasoline vehicles when combined (total traffic count) compared to when considered individually may signal a role for the interaction of their emissions as a determinant of on-road ROS in this pilot study. If further validated, this should not be overlooked in studies of on- or near-road particle exposure and its potential health effects.

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Atmospheric nanoparticles are one of those pollutants currently unregulated through ambient air quality standards. The aim of this chapter is to assess the environmental and health impacts of atmospheric nanoparticles in European environments. The chapter begins with the conventional information on the origin of atmospheric nanoparticles, followed by their physical and chemical characteristics. A brief overview of recently published review articles on this topic is then presented to guide those readers interested in exploring any specific aspect of nanoparticles in greater detail. A further section reports a summary of recently published studies on atmospheric nanoparticles in European cities. This covers a total of about 45 sampling locations in 30 different cities within 15 European countries for quantifying levels of roadside and urban background particle number concentrations (PNCs). Average PNCs at roadside and urban background sites were found to be 3.82±3.25 ×104 cm–3 and 1.63±0.82 ×104 cm–3, respectively, giving a roadside to background PNC ratio of ~2.4. Engineered nanoparticles are one of the key emerging categories of airborne nanoparticles, especially for the indoor environments. Their ambient concentrations may increase in future due to widespread use of nanotechnology integrated products. Evaluation of their sources and probable impacts on air quality and human health are briefly discussed in the following section. Respiratory deposition doses received by the public exposed to roadside PNCs in numerous European locations are then estimated. These were found to be in the 1.17–7.56 1010 h–1 range over the studied roadside European locations. The following section discusses the potential framework for airborne nanoparticle regulations in Europe and, in addition, the existing control measures to limit nanoparticle emissions at source. The chapter finally concludes with a synthesis of the topic areas covered and highlights important areas for further work.

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Recent research has described the restructuring of particles upon exposure to organic vapours; however, as yet hypotheses able to explain this phenomenon are limited. In this study, a range of experiments were performed to explore different hypotheses related to carbonaceous particle restructuring upon exposure to organic and water vapours, such as: the effect of surface tension, the role of organics in flocculating primary particles, as well as the ability of vapours to “wet” the particle surface. The change in mobility diameter (dm) was investigated for a range carbonaceous particle types (diesel exhaust, petrol exhaust, cigarette smoke, candle smoke, particles generated in a heptane/toluene flame, and wood smoke particles) exposed to different organic (heptane, ethanol, and dimethyl sulfoxide/water (1:1 vol%) mixture) and water vapours. Particles were first size-selected and then bubbled through an impinger (bubbler) containing either an organic solvent or water, where particles trapped inside rising bubbles were exposed to saturated vapours of the solvent in the impinger. The size distribution of particles was simultaneously measured upstream and downstream from the impinger. A size-dependent reduction in dm was observed when bubbling diesel exhaust, particles generated in a heptane/toluene flame, and candle smoke particles through heptane, ethanol and a dimethyl sulfoxide/water (1:1 vol %) mixture. In addition, the size distributions of particles bubbled through an impinger were broader. Moreover, an increase of the geometric standard deviation (σ) of the size distributions of particles bubbled through an impinger was also found to be size-dependent. Size-dependent reduction in dm and an increase of σ indicate that particles undergo restructuring to a more compact form, which was confirmed by TEM analysis. However, bubbling of these particles through water did not result in a size-dependent reduction in dm, nor in an increase of σ. Cigarette smoke, petrol exhaust, and wood smoke particles did not result in any substantial change in dm, or σ, when bubbled through organic solvents or water. Therefore, size-dependent reduction in the dm upon bubbling through organic solvents was observed only for particles that had a fractal-like structure, whilst particles that were liquid or were assumed to be spherical did not exhibit any reduction in dm. Compaction of fractal-like particles was attributed to the ability of condensing vapours to efficiently wet the particles. Our results also show that the presence of an organic layer on the surface of fractal-like particles, or the surface tension of the condensed liquid do not influence the extent of compaction.

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Quantifying spatial and/or temporal trends in environmental modelling data requires that measurements be taken at multiple sites. The number of sites and duration of measurement at each site must be balanced against costs of equipment and availability of trained staff. The split panel design comprises short measurement campaigns at multiple locations and continuous monitoring at reference sites [2]. Here we present a modelling approach for a spatio-temporal model of ultrafine particle number concentration (PNC) recorded according to a split panel design. The model describes the temporal trends and background levels at each site. The data were measured as part of the “Ultrafine Particles from Transport Emissions and Child Health” (UPTECH) project which aims to link air quality measurements, child health outcomes and a questionnaire on the child’s history and demographics. The UPTECH project involves measuring aerosol and particle counts and local meteorology at each of 25 primary schools for two weeks and at three long term monitoring stations, and health outcomes for a cohort of students at each school [3].