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Characterisation of the Chemical Properties and Behaviour of Aerosols in the Urban Environment

Young, Dominique Emma

[Thesis]. Manchester, UK: The University of Manchester; 2014.

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Abstract

Atmospheric aerosols have adverse effects on human health, air quality, and visibility and frequently result in severe pollution events, particularly in urban areas. However, the sources of aerosols and the processes governing their behaviour in the atmosphere, including those which lead to high concentrations, are not well understood thus limit our ability to accurately assess and forecast air quality.Presented here are the first long-term chemical composition measurements from an urban environment using an Aerodyne compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS). Organic aerosols (OA) were observed to account for a significant fraction (44%) of the total non-refractory submicron mass during 2012 at the urban background site in North Kensington, London, followed by nitrate (28%), sulphate (14%), ammonium (13%), and chloride (1%). The sources and components of OA were determined using Positive Matrix Factorisation (PMF) and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2), where HOA, COA, and SFOA were observed to be of equal importance across the year. The concentration of secondary OA increased during the summer yet the extent of oxidation, as defined by the oxygen content, showed no variability during the year.The main factors governing the diurnal, monthly, and seasonal trends observed in all organic and inorganic species were meteorological conditions, specific nature of the sources, and availability of precursors. Regional and transboundary pollution influenced total aerosol concentrations and high concentration events were observed to be governed by different factors depending on season. High-Resolution ToF-AMS measurements were used to further probe OA behaviour, where two SFOA factors were derived from PMF analysis in winter, which likely represent differences in burn conditions. In the summer an OA factor was identified, likely of primary origin, which was observed to be strongly associated with organic nitrates and anthropogenic emissions.This work uses instruments and techniques that have not previously been used in this way in an urban environment, where the results further the understanding of the chemical components of urban aerosols. Aerosol sources are likely to change in the future with increases in solid fuel burning as vehicular emissions decrease, with significant implications on air quality and health. Thus it is important to understand aerosol sources and behaviour in order to develop effective pollution abatement strategies.

Bibliographic metadata

Type of resource:
Content type:
Form of thesis:
Type of submission:
Degree type:
Doctor Of Philosophy
Degree programme:
PhD Atmospheric Sciences
Publication date:
Location:
Manchester, UK
Total pages:
246
Abstract:
Atmospheric aerosols have adverse effects on human health, air quality, and visibility and frequently result in severe pollution events, particularly in urban areas. However, the sources of aerosols and the processes governing their behaviour in the atmosphere, including those which lead to high concentrations, are not well understood thus limit our ability to accurately assess and forecast air quality.Presented here are the first long-term chemical composition measurements from an urban environment using an Aerodyne compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS). Organic aerosols (OA) were observed to account for a significant fraction (44%) of the total non-refractory submicron mass during 2012 at the urban background site in North Kensington, London, followed by nitrate (28%), sulphate (14%), ammonium (13%), and chloride (1%). The sources and components of OA were determined using Positive Matrix Factorisation (PMF) and attributed as hydrocarbon-like OA (HOA), cooking OA (COA), solid fuel OA (SFOA), type 1 oxygenated OA (OOA1), and type 2 oxygenated OA (OOA2), where HOA, COA, and SFOA were observed to be of equal importance across the year. The concentration of secondary OA increased during the summer yet the extent of oxidation, as defined by the oxygen content, showed no variability during the year.The main factors governing the diurnal, monthly, and seasonal trends observed in all organic and inorganic species were meteorological conditions, specific nature of the sources, and availability of precursors. Regional and transboundary pollution influenced total aerosol concentrations and high concentration events were observed to be governed by different factors depending on season. High-Resolution ToF-AMS measurements were used to further probe OA behaviour, where two SFOA factors were derived from PMF analysis in winter, which likely represent differences in burn conditions. In the summer an OA factor was identified, likely of primary origin, which was observed to be strongly associated with organic nitrates and anthropogenic emissions.This work uses instruments and techniques that have not previously been used in this way in an urban environment, where the results further the understanding of the chemical components of urban aerosols. Aerosol sources are likely to change in the future with increases in solid fuel burning as vehicular emissions decrease, with significant implications on air quality and health. Thus it is important to understand aerosol sources and behaviour in order to develop effective pollution abatement strategies.
Thesis main supervisor(s):
Thesis co-supervisor(s):
Thesis advisor(s):
Language:
en

Institutional metadata

University researcher(s):

Record metadata

Manchester eScholar ID:
uk-ac-man-scw:238054
Created by:
Young, Dominique
Created:
27th October, 2014, 17:33:35
Last modified by:
Young, Dominique
Last modified:
16th November, 2017, 14:24:46

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