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Discussion papers
https://doi.org/10.5194/acp-2018-1151
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2018-1151
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 16 Nov 2018

Research article | 16 Nov 2018

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This discussion paper is a preprint. A revision of this manuscript was accepted for the journal Atmospheric Chemistry and Physics (ACP) and is expected to appear here in due course.

The EMEP Intensive Measurement Period campaign, 2008–2009: Characterizing the carbonaceous aerosol at nine rural sites in Europe

Karl Espen Yttri1, David Simpson2,3, Robert Bergström3,4, Gyula Kiss5, Sönke Szidat6, Darius Ceburnis7, Sabine Eckhardt1, Christoph Hueglin8, Jacob Klenø Nøjgaard9, Cinzia Perrino10, Ignacio Pisso1, Andre Stephan Henry Prevot11, Jean-Philippe Putaud12, Gerald Spindler13, Milan Vana14, Yan-Lin Zhang10,11,13, and Wenche Aas1 Karl Espen Yttri et al.
  • 1NILU – Norwegian Institute for Air Research (NILU), 2027 Kjeller, Norway
  • 2Norwegian Meteorological Institute, 0313 Oslo, Norway
  • 3Department of Space, Earth and Environment, Chalmers University of Technology, 41296 Gothenburg
  • 4Swedish Meteorological and Hydrological Institute, 60176 Norrköping, Sweden
  • 5MTA-PE Air Chemistry Research Group, 8200 Veszprém – Hungary
  • 6Department of Chemistry and Biochemistry & Oeschger Centre for Climate Change Research, University of Bern, 3012 Berne, Switzerland
  • 7School of Physics and Centre for Climate and Air Pollution Studies, Ryan Institute, National University of Ireland Galway, Galway, Ireland
  • 8EMPA, 8600 Duebendorf, Switzerland
  • 9National Environmental Research Institute, 4000 Roskilde, Denmark
  • 10CNR – Institute of Atmospheric Pollution Research, 00015 Monterotondo Stazione (Rome), Italy
  • 11Paul Scherrer Institut, 5232 Villigen-PSI, Switzerland
  • 12European Commission, Joint Research Centre, 21027 Ispra (VA), Italy
  • 13Leibniz Institute for Tropospheric Research, 04318 Leipzig, Germany
  • 14The Czech Hydrometeorological Institute (CHMI), Prague, Czech Republic

Abstract. Source apportionment (SA) of carbonaceous aerosol was performed as part of the EMEP Intensive Measurement Periods (EIMPs), conducted in fall 2008 and winter/spring 2009. Levels of elemental carbon (EC), particulate organic carbon (OCp), particulate total carbon (TCp), levoglucosan and 14C in PM10, observed at nine European rural background sites, were used as input for the SA, whereas Latin Hypercube Sampling (LHS) was used to statistically treat the multitude of possible combinations resulting when ambient concentrations were combined with appropriate emission ratios. Five predefined sources/subcategories of carbonaceous aerosol were apportioned: Elemental and organic carbon from combustion of biomass (ECbb and OCbb) and from fossil fuel (ECff and OCff) sources, as well as remaining non-fossil organic carbon (OCrnf), typically dominated by natural sources.

The carbonaceous aerosol concentration decreased from South to North, as did the concentration of the apportioned carbonaceous aerosol. OCrnf was more abundant in fall compared to winter/spring, reflecting the vegetative season, and made a larger contribution to TCp than anthropogenic sources (here: ECbb, OCbb, ECff and OCff) at four of the sites, whereas anthropogenic sources dominated at all but one sites in winter/spring. Levels of OCbb and ECbb were typically higher in winter/spring than in fall, due to larger residential wood burning emissions in the heating season, whereas there was no consistent seasonal pattern for fossil fuel emissions. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the Central European sites in fall, whereas fossil fuel sources dominated at the southernmost and the two northernmost sites. In winter/spring, biomass burning was the major anthropogenic source at all but two sites. Addressing EC in particular, fossil fuel sources dominated at all sites in fall, whereas there was as shift towards biomass burning in winter/spring for the southernmost sites. Influence of residential wood burning emissions was substantial already in the first week of sampling in fall, constituting 30–50 % of TCp at most sites, showing that this source can be dominating even at a time of the year when the ambient temperature in Europe is still rather high.

Model calculations were made, attempting to reproduce LHS-derived OCbb and ECbb, using two different residential wood burning emission inventories. Both simulations strongly under-predicted the LHS-derived values at most sites outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential combustion (and including intermediate volatility compounds, IVOC) improved model results at most sites compared to the base-case emissions (based mainly on officially reported national emissions), but at the three southernmost sites the modelled OCbb and ECbb concentrations were still much lower than the LHS source apportioned results.

The current study shows that natural sources is a major contributor to the carbonaceous aerosol in Europe even in fall and in winter/spring, and that residential wood burning emissions can be equally large or larger than that of fossil fuel sources, depending on season and region. Our results suggest that residential wood burning emissions are still poorly constrained for large parts of Europe. The need to improve emission inventories is obvious, with harmonization of emission factors between countries likely being the most important step to improve model calculations, not only for biomass burning emissions, but for European PM2.5 concentrations in general.

Karl Espen Yttri et al.
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Interactive discussion
Status: closed
Status: closed
AC: Author comment | RC: Referee comment | SC: Short comment | EC: Editor comment
Printer-friendly Version - Printer-friendly version Supplement - Supplement
Karl Espen Yttri et al.
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Short summary
Carbonaceous aerosol from natural sources were abundant regardless of season. Residential wood burning (RWB) emissions were occasionally equally large or larger than that of fossil fuel sources, depending on season and region. RWB emissions are poorly constrained, thus emissions inventories need improvement. To harmonize emission factors between countries is likely the most important step to improve model calculations for biomass burning emissions and European PM2.5 concentrations in general.
Carbonaceous aerosol from natural sources were abundant regardless of season. Residential wood...
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