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Titel |
Investigations of primary and secondary particulate matter of different wood combustion appliances with a high-resolution time-of-flight aerosol mass spectrometer |
VerfasserIn |
M. F. Heringa, P. F. DeCarlo, R. Chirico, T. Tritscher, J. Dommen, E. Weingärtner, Rene Richter, G. Wehrle, A. S. H. Prévôt, U. Baltensperger |
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 ; 11, no. 12 ; Nr. 11, no. 12 (2011-06-23), S.5945-5957 |
Datensatznummer |
250009867
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Publikation (Nr.) |
copernicus.org/acp-11-5945-2011.pdf |
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Zusammenfassung |
A series of photo-oxidation smog chamber experiments were performed to
investigate the primary emissions and secondary aerosol formation from two
different log wood burners and a residential pellet burner under different
burning conditions: starting and flaming phase. Emissions were sampled from
the chimney and injected into the smog chamber leading to primary organic
aerosol (POA) concentrations comparable to ambient levels. The composition
of the aerosol was measured by an Aerodyne high resolution time-of-flight
aerosol mass spectrometer (HR-TOF-AMS) and black carbon (BC)
instrumentation. The primary emissions were then exposed to xenon light to
initiate photo-chemistry and subsequent secondary organic aerosol (SOA)
production. After correcting for wall losses, the average increase in
organic matter (OM) concentrations by SOA formation for the starting and
flaming phase experiments with the two log wood burners was found to be a
factor of 4.1±1.4 after five hours of aging. No SOA formation was
observed for the stable burning phase of the pellet burner. The startup
emissions of the pellet burner showed an increase in OM concentration by a
factor of 3.3. Including the measured SOA formation potential, average
emission factors of BC+POA+SOA, calculated from CO2 emission, were
found to be in the range of 0.04 to 3.9 g/kg wood for the stable burning
pellet burner and an old log wood burner during startup respectively. SOA
contributed significantly to the ion C2H4O2+ at mass to
charge ratio m/z 60, a commonly used marker for primary emissions of wood
burning. This contribution at m/z 60 can overcompensate for the degradation of
levoglucosan leading to an overestimation of the contribution of wood
burning or biomass burning to the total OM. The primary organic emissions
from the three different burners showed a wide range in O:C atomic ratio
(0.19−0.60) for the starting and flaming conditions, which also increased
during aging. Primary wood burning emissions have a rather low relative
contribution at m/z 43 (f 43) to the total organic mass spectrum. The
non-oxidized fragment C3H7+ has a considerable contribution
at m/z 43 for the fresh OA with an increasing contribution of the oxygenated
ion C2H3O+ during aging. After five hours of aging, the OA
has a rather low C2H3O+ signal for a given CO2+
fraction, possibly indicating a higher ratio of acid to non-acid oxygenated
compounds in wood burning OA compared to other oxygenated organic aerosol (OOA). |
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