Biomedical subjects
N Carslaw
Publications and source records attributed to N Carslaw.
Measurement and modelling of air pollution and atmospheric chemistry in the U.K. West Midlands conurbation: overview of the PUMA Consortium project.
The PUMA (Pollution of the Urban Midlands Atmosphere) Consortium project involved intensive measurement campaigns in the Summer of 1999 and Winter of 1999/2000, respectively, in which a wide variety of air pollutants were measured in the UK West Midlands conurbation including detailed speciation of VOCs and major component analysis of aerosol. Measurements of the OH and HO2 free radicals by the FAGE technique demonstrated that winter concentrations of OH were approximately half of those measured during the summer despite a factor of 15 reduction in production through the photolysis of ozone. Detailed box modelling of the fast reaction chemistry revealed the decomposition of Criegee intermediates formed from ozone-alkene reactions to be responsible for the majority of the formation of hydroxyl in both the summer and winter campaigns, in contrast to earlier rural measurements in which ozone photolysis was predominant. The main sinks for hydroxyl are reactions with NO2, alkenes and oxygenates. Concentrations of the more stable hydrocarbons were found to be relatively invariant across the conurbation, but the impacts of photochemistry were evident through analyses of formaldehyde which showed the majority to be photochemical in origin as opposed to emitted from road traffic. Measurements on the upwind and downwind boundaries of the conurbation revealed substantial enhancements in NOx as a result of emissions within the conurbation, especially during westerly winds which carried relatively clean air. Using calcium as a tracer for crustal particles, it proved possible to reconstruct aerosol mass from the major chemical components with a fairly high degree of success. The organic to elemental carbon ratios showed a far greater influence of photochemistry in summer than winter, presumably resulting mainly from the greater availability of biogenic precursors during the summer campaign. Two urban airshed models were developed and applied to the conurbation, one Eulerian, the other Lagrangian. Both were able to give a good simulation of concentrations of both primary and secondary pollutants at urban background locations.
A larger pool of ozone-forming carbon compounds in urban atmospheres
Volatile organic compounds play a central role in the processes that generate both urban photochemical smog and tropospheric ozone. For successful and accurate prediction of these pollution episodes, identification of the dominant reactive species within the volatile organic carbon pool is needed. At present, lack of resolution inherent in single-column chromatographic analysis limits such a detailed chemical characterization of the complex urban atmosphere. Here we present an improved method of peak deconvolution from double-column (orthogonal) gas chromatography. This has enabled us to isolate and classify more than 500 chemical species of volatile organic compounds in urban air, including over 100 multi-substituted monoaromatic and volatile oxygenated hydrocarbons. We suggest that previous assessments of reactive carbon species may therefore have underestimated the contribution made by volatile organic compounds to urban pollution, particularly for compounds with more than six carbon atoms. Incorporating these species in predictive models should greatly improve our understanding of photochemical ozone yields and the formation of harmful secondary organic aerosols.