Biomedical subjects

Roy M Harrison

Publications and source records attributed to Roy M Harrison.

13 recordsLinked to original sources

PubMed2006

Single-particle detection efficiencies of aerosol time-of-flight mass spectrometry during the North Atlantic marine boundary layer experiment.

During the North Atlantic marine boundary layer experiment (NAMBLEX) sampling campaign at Mace Head, Ireland, both continental and maritime air masses were sampled. Aerosol was characterized both with a TSI 3800 time-of-flight mass spectrometer (ATOFMS) and a MOUDI microorifice impactor, and particle number counts were measured independently with an aerodynamic particle sizer. The data have been analyzed in order to elucidate factors determining the particle detection efficiencies of the ATOFMS. These are broken down according to the efficiency of the inlet system, the hit efficiency on particles which enter the sensing zone of the instrument and the sensitivity of the measured ion signal to the chemical species. A substantial matrix effect depending on the chemical composition of the aerosol sampled at the time was found, which is reflected in variations in the hit efficiency of particles entering the sensing zone of the instrument with the main desorption-ionization laser. This is in addition to the strong inverse power-law dependence of inlet transmission efficiency on particle diameter. The variation in hit efficiency with particle type is likely attributable to differences in the energetics of laser energy absorption, ablation, and ion formation. However, once variations in both inlet transmission and hit efficiencies are taken into account, no additional matrix dependence of ATOFMS response is required to obtain a linear relationship between the ion signal and the concentration of a particular chemical species. The observations show that a constant mass of material is ionized from each particle, irrespective of size. Consequently the integrated ion signal for a given chemical component and particle size class needs to be increased by a factor related to the cube of particle diameter in order to correlate with the airborne mass of that component.

Aerosols↗

PubMed2006

An analysis of spatial and temporal properties of daily sulfate, nitrate and chloride concentrations at UK urban and rural sites.

Daily measurements of sulfate, nitrate and chloride in PM(10) have been made at three geographically separated UK sites over a three year period. Chloride shows a clear seasonal pattern with highest concentrations in winter, whilst sulfate and nitrate both show highest concentrations in the spring, apparently related to weather patterns. Spatial variability of both sulfate and nitrate is low in comparison to temporal variations, with high correlations of both species between all three sites, London (North Kensington), Harwell and Belfast, despite a geographic separation of 510 km. Both SO/SO(2) and NO/NO(x) ratios are considerably higher in summer than winter, reflecting a greater oxidising capacity of the atmosphere. SO(4)(2-)/NO(3)(-) ratios are higher in summer than winter, suggesting that aqueous phase oxidation of SO(2), expected to be most important in the winter months is not appreciably influencing production of sulfate aerosol, although greater dissociation of ammonium nitrate in summer may also play a role. Regression of concentrations at London, North Kensington with those from the proximate rural site of Harwell is interpreted as showing a similar effect of regional transport at the two sites and a small influence of local formation in the urban atmosphere or primary emissions, averaging 0.46 microg m(-3) of nitrate and 0.22 microg m(-3) of sulfate.

Aerosols↗

PubMed2006

Particulate sulphate and nitrate in Southern England and Northern Ireland during 2002/3 and its formation in a photochemical trajectory model.

Daily measurements of sulphate and nitrate are reported from Harwell in southern England and Belfast in Northern Ireland for the period 2002/3. When the higher percentiles are compared with the mean concentration, nitrate reveals considerably greater episodicity than either sulphate or PM(10) (measured by TEOM). A photochemical trajectory model using the Master Chemical Mechanism scheme has been used to predict daily concentrations of both nitrate and sulphate aerosol over the period March to August 2002 at the Belfast and Harwell sites. This has been carried out for daily samples using 72, 96 and 120 h air mass back trajectories obtained from both the British Atmospheric Data Centre and the HYSPLIT on-line service. Additionally, model simulations have been conducted for 5 trajectories generated through clustering of the trajectories for individual days. This reveals an under-prediction of the model associated particularly with trajectories originating from the European mainland. In general, the model performs reasonably well in simulating concentrations of both nitrate and sulphate, which is surprising given that the model does not account for processes requiring the presence of liquid water. This suggests that aqueous phase oxidation processes may not make a major contribution to airborne sulphate concentrations in the U.K. in the spring and summer months. It appears that inclusion of explicit ammonium nitrate formation chemistry may be essential to reliable prediction of episodic nitrate peaks.

Aerosols↗

PubMed2006

Trace metal concentrations and water solubility in size-fractionated atmospheric particles and influence of road traffic.

The abundance and the behavior of metals (Al, Ti, Mn, Fe, Co, Ni, Cu, Zn, Se, Ag, Cd, Sn, Ba, Pt, Hg, and Pb) and ions (Na+ K+ Mg2+ Ca2+, NH4+, Cl-, NO3-, SO4(2-), PO4(3-), and oxalate) in size-fractionated atmospheric particulate matter (PM) were studied in the U. K. and Ireland at four observation sites simulating extreme degrees of vehicular-traffic influence in the environment. Trace metals in urban PM showed distinct types of size-fractionated behavior depending on the particle sources from which they originate. In coarse PM (1.5 < Dp < 3.0 microm) the concentrations of copper, barium, and iron correlated closely across over 2 orders of magnitude in urban air, which is seen as evidence that major portions of transition metals (Cu, Ba, Fe, and Mn) are released through abrasive vehicular emissions, particularly the wear of brake linings. Further results are strongly indicative of a decoupling of coarse iron and calcium, the former arising predominantly from vehicles, the latter from soil resuspension. In fine PM (Dp < 0.5 microm), several combustion and secondary sources of particulates were identified, but these were much less unique in terms of elemental fingerprints. An analysis of the water solubility of trace metals yielded that solubility varies considerably with element and, to a lesser extent, with particle size. Notable differences were found to the elemental water solubilities determined in previous work, partially explained by differences in extraction procedures.

Air Pollutants↗

PubMed2005

Model simulation of meteorology and air quality during the summer PUMA intensive measurement campaign in the UK West Midlands conurbation.

The Regional Atmospheric Modeling System (RAMS) and Urban Airshed Model (UAM IV) have been implemented for prediction of air pollutant concentrations within the West Midlands conurbation of the United Kingdom. The modelling results for wind speed, direction and temperature are in reasonable agreement with observations for two stations, one in a rural area and the other in an urban area. Predictions of surface temperature are generally good for both stations, but the results suggest that the quality of temperature prediction is sensitive to whether cloud cover is reproduced reliably by the model. Wind direction is captured very well by the model, while wind speed is generally overestimated. The air pollution climate of the UK West Midlands is very different to those for which the UAM model was primarily developed, and the methods used to overcome these limitations are described. The model shows a tendency towards under-prediction of primary pollutant (NOx and CO) concentrations, but with suitable attention to boundary conditions and vertical profiles gives fairly good predictions of ozone concentrations. Hourly updating of chemical concentration boundary conditions yields the best results, with input of vertical profiles desirable. The model seriously underpredicts NO2/NO ratios within the urban area and this appears to relate to inadequate production of peroxy radicals. Overall, the chemical reactivity predicted by the model appears to fall well below that occurring in the atmosphere.

Air Pollutants↗

PubMed2005

Fine (PM2.5) and coarse (PM2.5-10) particulate matter on a heavily trafficked London highway: sources and processes.

A large dataset for PM2.5 and PMcoarse (PM2.5-10) concentrations monitored near a busy London highway (Marylebone Road) has been analyzed to define the factors that lead to high concentrations. The following have been highlighted as major influencing parameters: wind speed, prevailing wind direction (because of its role on the microscale dispersion within the street), the daily cycle of the atmospheric boundary layer (stable during the night/ convective and mixed during the day), and traffic density. The mainly diesel heavy-duty vehicles are the main source of fine particulate matter at Marylebone Road. In particular, lorries (trucks) dominate PM10 exhaust emissions which are mainly in the fine (<2.5 microm) size range. A strong correlation with PMcoarse suggests that the heavy-duty traffic is largely responsible for this component also. Substantial local increments in PM2.5 and PMcoarse due to traffic have been estimated and a large part of the increment in PMcoarse concentrations is inferred to arise from resuspended road dust emissions since the contribution of abrasion processes estimated from emission factors is modest. Despite the strong influence of traffic on PM concentrations measured at Marylebone Road the analysis of factors leading to the highest 5% of hourly concentrations of PM10 at Marylebone Road reveals that almost half of these events were due to building works. The other events occurred when all or most of the key factors occurred simultaneously (heavy traffic, poor dispersion, etc.). Some episodes of high PM2.5 concentrations were associated with long-range transport in which the regional PM2.5 constituted most of the local concentrations.

Air Pollutants↗

PubMed2005

Multisite study of particle number concentrations in urban air.

Particle number concentration data are reported from a total of eight urban site locations in the United Kingdom. Of these, six are central urban background sites, while one is an urban street canyon (Marylebone Road) and another is influenced by both a motorway and a steelworks (Port Talbot). The concentrations are generally of a similar order to those reported in the literature, although higher than those in some of the other studies. Highest concentrations are at the Marylebone Road site and lowest are at the Port Talbot site. The central urban background locations lie somewhere between with concentrations typically around 20 000 cm(-3). A seasonal pattern affects all sites, with highest concentrations in the winter months and lowest concentrations in the summer. Data from all sites show a diurnal variation with a morning rush hour peak typical of an anthropogenic pollutant. When the dilution effects of windspeed are accounted for, the data show little directionality at the central urban background sites indicating the influence of sources from all directions as might be expected if the major source were road traffic. At the London Marylebone Road site there is high directionality driven by the air circulation in the street canyon, and at the Port Talbot site different diurnal patterns are seen for particle number count and PM10 influenced by emissions from road traffic (particle number count) and the steelworks (PM10) and local meteorological factors. Hourly particle number concentrations are generally only weakly correlated to NO(x) and PM10, with the former showing a slightly closer relationship. Correlations between daily average particle number count and PM10 were also weak. Episodes of high PM10 concentration in summer typically show low particle number concentrations consistent with transport of accumulation mode secondary aerosol, while winter episodes are frequently associated with high PM10 and particle number count arising from poor dispersion of local primary emissions.

Air Pollutants↗

PubMed2005

Characterization of humic substances by environmental scanning electron microscopy.

Environmental scanning electron microscopy (ESEM) is a new technique capable of imaging micron and submicron particles. Here, we have applied it to image and quantify natural aquatic organic matter (standard Suwannee River humic acid, SRHA). Uniquely, we have observed the humic aggregate structures as a function of humidity and pH. Large aggregates of tens of micrometers were observed as the dominant material under all conditions, although much smaller material was also observed. Fractal dimensions (D) were calculated between 1.48 and 1.70, although these values were not statistically different under conditions of low humidity. However, D values calculated at high humidities (85%) during the rehydration phase were significantly lower (1.48+/-0.01) than in the initial dehydration phase (1.69+/-0.01). This hysteresis indicated that full rehydration of the HS was either kinetically slow or irreversible after dehydration. Fractal analysis of ESEM images was also performed to probe the change in aggregate structure as a function of pH. Minimum values were calculated at neutral pHs, rising by 0.1-0.2 at both high and low pHs because of a combination of the physical chemistry of HS and the impacts of the drying regime within the ESEM. Thus, ESEM was an important complementary technique to other analytical methods. At present, ESEM cannot be used to image nonperturbed natural samples. However, the method is an ideal method for probing the changes in colloid structure as function of hydration state and has the potential to perform fully quantitative and nonperturbing analysis of colloidal structure.

Chemistry Techniques, Analytical↗

PubMed2004

Key pollutants--airborne particles.

The sources and composition of airborne particles, and trends observed over the past 50 years are reviewed in this paper. Major components of recent samples include elemental and organic carbon, secondary ammonium sulphate and ammonium nitrate, resuspended dust, and soil and sodium chloride. Early measurements employed the black smoke technique. More recently, PM(10) has been the accepted measure and is the basis for air quality standards and limit values. Between 1970 and 1999, a substantial reduction in emissions of particulate matter was achieved mainly through a cut in emissions from commercial, residential, and institutional combustion. Forthcoming European Union standards are likely to require particulate traps on new diesel vehicles.

Journal Article↗

PubMed2004

Climate factors influencing bacterial count in background air samples.

Total (as opposed to culturable) bacterial number counts are reported for four sites in the United Kingdom measured during campaigns over four separate seasons. These are interpreted in relation to simple climatic factors, i.e. temperature, wind speed and wind direction. Temperature has a marked effect at all four sites with data for a rural coastal site conforming best to a simple exponential model. Data for the other rural and urban locations show a baseline similar to that determined at the coastal rural location, but with some very significant positive excursions. The temperature dependence of bacterial number is found to conform to that typical of bacterial growth rates. At the coastal rural location, bacterial numbers normalised for temperature show no dependence on wind speed whilst at the inland sites there is a decrease with increasing wind speed of the form expected for a large area source. Only one site appeared to show a systematic relationship of bacterial concentrations to wind direction that being a site in the suburbs of Birmingham with highest number concentrations observed on a wind sector approaching from the city centre. PCR techniques have been used to identify predominant types of bacteria and results are presented which show that Bacillus was the dominant genus observed at the three inland sites during the winter and summer seasons. Pseudomonas appeared with comparable frequency at certain sites and seasons. There was in general a greater diversity of bacteria at the coastal site than at the inland sites.

Air Microbiology↗

PubMed2004

The effects of meteorological factors on atmospheric bioaerosol concentrations--a review.

Over land surfaces a quarter of the total airborne particulate may be made up of biological material in the form of pollen, fungal spores, bacteria, viruses, or fragments of plant and animal matter. Meteorological variables affect the initial release of this material and its dispersal once airborne. Temperature and water availability will affect the size of the source and will control the release of some actively released fungal spores. Inertly released material will become airborne when the drying of the surface reduces bonding forces, and when the material is disrupted by sufficiently strong air movement or by mechanical disturbance. The wind speed necessary to disrupt material is noted to be less on a plant surface than on the ground surface. Measurements of the concentrations of airborne material near dominant sources are reviewed for both area sources, and for point sources such as sewage and waste treatment works, agricultural practices, and diseased animals. The concentration of airborne material remote from sources is considered along with the effects of on and off shore winds and some examples of long distance transport of material. The vertical concentration of bacteria is noted to decline less rapidly than that of fungal spores. The short-term variation of pollen, fungal spore, and bacterial concentrations are also considered.

Aerosols↗

PubMed2004

Correlations in the chemical composition of rural background atmospheric aerosol in the UK determined in real time using time-of-flight mass spectrometry.

An aerosol time-of-flight mass spectrometer (ATOFMS) was used to determine, in real time, the size and chemical composition of individual particles in the atmosphere at the remote inland site of Eskdalemuir, Scotland. A total of 51,980 particles, in the size range 0.3-7.4 microm, were detected between the 25th and 30th June 2001. Rapid changes in the number density, size and chemical composition of the atmospheric aerosol were observed. These changes are attributed to two distinct types of air mass; a polluted air mass that had passed over the British mainland before reaching Eskdalemuir, interposed between two cleaner air masses that had arrived directly from the sea. Such changes in the background aerosol could clearly be very important to studies of urban aerosols and attempts at source apportionment. The results of an objective method of data analysis are presented. Correlations were sought between the occurrence of: lithium, potassium, rubidium, caesium, beryllium, strontium, barium, ammonium, amines, nitrate, nitrite, boron, mercury, sulfate, phosphate, fluorine, chlorine, bromine, iodine and carbon (both elemental and organic hydrocarbon) in both fine (d < 2.5 microm) and coarse (d > 2.5 microm) particle fractions. Several previously unreported correlations were observed, for instance between the elements lithium, beryllium and boron. The results suggest that about 2 in 3 of all fine particles (by number rather than by mass), and 1 in 2 of all coarse particles containing carbon, consisted of elemental carbon rather than organic hydrocarbon (although a bias in the sensitivity of the ATOFMS could have affected these numbers). The ratio of the number of coarse particles containing nitrate anions to the number of particles containing chloride anions exceeded unity when the air mass had travelled over the British mainland. The analysis also illustrates that an air mass of marine origin that had travelled slowly over agricultural land can accumulate amines and ammonium.

Aerosols↗

PubMed2002

Levels and sources of personal inhalation exposure to volatile organic compounds.

Personal exposures to VOCs of 12 urban dwellers were measured directly via personal monitoring and indirectly via static monitoring combined with personal activity diaries. Over 5-10 days, day-to-day variations in personal exposures of individuals were substantial, with statistically significant (p<0.05) deviation from the normal distribution observed for daily exposures to one or more VOCs for several subjects. Daytime concentrations generally exceeded night time, with day:night mean concentration ratios for each sampling day >1 for most VOCs, with the maximum (3.85) occurring for 1,3-butadiene. Exposure in the home contributed 50-80% of overall individual exposure to 1,3-butadiene and benzene. For most VOCs, while absolute values of direct and indirect exposure estimates were significantly different (p<0.05), linear regression of direct and indirect exposure estimates revealed statistically significant correlation (p<0.01), confirming previous observations that indirect monitoring can provide satisfactory estimates of personal inhalation exposure to VOCs. ETS, the use of vehicles, and heating (but not cooking) all made appreciable contributions to personal exposure to all target VOCs.

Air Pollutants↗