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Titel |
Contributions from transport, solid fuel burning and cooking to primary organic aerosols in two UK cities |
VerfasserIn |
J. D. Allan, P. I. Williams, W. T. Morgan, C. L. Martin, M. J. Flynn, J. Lee, E. Nemitz, G. J. Phillips, M. W. Gallagher, H. Coe |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 10, no. 2 ; Nr. 10, no. 2 (2010-01-22), S.647-668 |
Datensatznummer |
250007967
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Publikation (Nr.) |
copernicus.org/acp-10-647-2010.pdf |
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Zusammenfassung |
Organic matter frequently represents the single largest fraction of fine
particulates in urban environments and yet the exact contributions from
different sources and processes remain uncertain, owing in part to its
substantial chemical complexity. Positive Matrix Factorisation (PMF) has
recently proved to be a powerful tool for the purposes of source attribution
and profiling when applied to ambient organic aerosol data from the Aerodyne
Aerosol Mass Spectrometer (AMS). Here we present PMF analysis applied to AMS
data from UK cities for the first time. Three datasets are analysed, with
the focus on objectivity and consistency. The data were collected in London
during the Regent's Park and Tower Environmental Experiment (REPARTEE)
intensives and Manchester. These occurred during the autumn and wintertime,
such that the primary fraction would be prominent. Ambiguities associated
with rotationality within sets of potential solutions are explored and the
most appropriate solution sets selected based on comparisons with external
data. In addition to secondary organic aerosols, three candidate sources of
primary organic aerosol (POA) were identified according to mass spectral and
diurnal profiles; traffic emissions, cooking and solid fuel burning (for
space heating). Traffic represented, on average, 40% of POA during
colder conditions and exhibited a hydrocarbon-like mass spectrum similar to
those previously reported. Cooking aerosols represented 34% of POA and
through laboratory work, their profile was matched with that sampled from
the heating of seed oils, rather than previously-published spectra derived
from charbroiling. This suggests that in these locations, oil from frying
may have contributed more to the particulate than the meat itself. Solid
fuel aerosols represented 26% of POA during cold weather conditions but
were not discernable during the first REPARTEE campaign, when conditions
were warmer than the other campaigns. This factor showed features associated
with biomass burning and occurred mainly at night. Grid-scale emission
factors of the combustion aerosols suitable for use in chemical transport
models were derived relative to CO and NOx. The traffic aerosols were
found to be 20.5 μg m−3 ppm−1 relative to CO for Manchester
and 31.6 μg m−3 ppm−1 relative to NOx for London. Solid
fuel emissions were derived as 24.7 μg m−3 ppm−1 relative to
CO for Manchester. These correspond to mass emission ratios of 0.018, 0.026
(as NO) and 0.021 respectively and are of a similar order to previously
published estimates, derived from other regions or using other approaches. |
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