DOUCE, David Stewart. (1998). Air quality assessment and the use of specific markers to apportion pollutants to source. Doctoral, Sheffield Hallam University (United Kingdom).. [Thesis]
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19672:454206
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10695712.pdf - Accepted Version
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10695712.pdf - Accepted Version
Available under License All rights reserved.
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Abstract
The contributions of specific polluting sources to both indoor and outdoor atmospheric pollution are difficult to determine, as solid and gaseous products from different combustion sources are often similar. Sometimes, however, a marker compound can be identified that is unique to a pollution source (or at least not present in most other local combustion sources) and which will allow assessment of the contribution of that source to total atmospheric pollution.The aim of this study was to identify suitable marker compounds and methods for the apportionment (assessment of percentage contribution) of specific sources to atmospheric pollution. The sources selected were diesel exhaust emissions in outdoor, and environmental tobacco smoke (ETS) in indoor environments. Studies with controlled (laboratory) atmospheres would be followed by field studies using these methods and markers to produce apportionments for these sources to air pollution in selected environments. Initial analysis of such polluting sources was therefore the qualitative analysis of volatile compounds and particulate associated material, both organic and inorganic. Volatile organic compounds were adsorbed onto various resins, while particulate material was sampled onto various filter paper types. Organics were determined by GC-AED and GC-MS, and elements by ICP-MS.1-Nitropyrene was identified as a suitable marker for diesel particulate emissions (<5um). A large volume air sample from Sheffield city centre using 1-nitropyrene as a marker suggested that 63% of atmospheric particulate material (<5um) might be of diesel origin. However the concentration of 1-nitropyrene is low in atmospheric samples, and in the volumes used in routine sampling the amount of 1-nitropyrene was below the limit of detection on the instrument used. In an alternative approach the aliphatic alkane tetracosane (C24) was used as a diesel marker for urban air, with a 1-nitropyrene:tetracosane ratio derived from the average results from laboratory experiments with a diesel engine running at various speeds and loads. This approach yielded apportionment values ranging from 5-85% for the diesel contribution to particulate material (<5mum) in the urban air of Sheffield. No volatile marker compound was found for diesel apportionment.The contribution of ETS to atmospheric pollution has previously been estimated from the measurement of respirable suspended particulates (RSP), which was superseded by total UV absorbance and total fluorescence of a methanol extract. More recent work has suggested the use of solanesol or scopoletin as marker compounds. This thesis shows that the non specific methods overestimated the particulate contribution of ETS in some atmospheres, and that solanesol is a better marker compound than scopoletin. Preliminary studies from a small number of smokers homes and offices, with solanesol as a marker compound for particulate ETS, indicated that ETS contributions to total particulate material (<5mum) ranged from 6 to 49% in homes and 11 to 28% in offices.Pyrrole was used as a marker for ETS contribution to volatile organic pollution, and studies with controlled atmospheres with a smoking machine allowed calculation of the ratios of pyrrole to other volatile organic compounds (VOC's) in ETS. Samples from the field study were used to produce apportionment percentage levels of benzene, toluene, o-xylene and p+m-xylene associated with ETS.In addition the use of tree bark as a atmospheric sink for airborne particulates was investigated. Six nitrated polycyclic aromatic hydrocarbons associated with diesel emissions were quantified in bark extracts and levels of these were found to be highest during winter months.
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