Atmos. Chem. Phys. Discuss., 8, 19561-19604, 2008
www.atmos-chem-phys-discuss.net/8/19561/2008/
doi:10.5194/acpd-8-19561-2008
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This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
The influence of traffic and wood combustion on the stable isotopic composition of carbon monoxide
M. Saurer, A. S. H. Prévôt, J. Dommen, J. Sandradewi, U. Baltensperger, and R. T. W. Siegwolf
Paul Scherrer Institut, 5232 Villigen PSI, Switzerland

Abstract. Carbon monoxide in the atmosphere is originating from various combustion and oxidation processes. Recently, the proportion of CO resulting from the combustion of wood for domestic heating may have increased due to political measures promoting this renewable energy source. Here, we used the stable isotope composition of CO (δ13C and δ18O) for the characterization of different CO sources in Switzerland, along with other indicators for traffic and wood combustion (NOx-concentration, aerosol light absorption at different wavelengths). We assessed diurnal variations of the isotopic composition of CO at 3 sites during winter: a village site dominated by domestic heating, a site close to a motorway and a rural site. The isotope ratios of wood combustion emissions were studied at a test facility, indicating significantly lower δ18O of CO from wood combustion compared to traffic emissions. At the village and the motorway site, we observed very pronounced diurnal δ18O-variations of CO with an amplitude of up to 8‰. Solving the isotope mass balance equation for three distinct sources (wood combustion, traffic, clean background air) resulted in diurnal patterns consistent with other indicators for wood burning and traffic. The average night-time contribution of wood-burning to total CO was 70% at the village site, 47% at the motorway site and 28% at the rural site based on the isotope mass balance. As this analysis showed a strong sensitivity towards the pure source isotope values, we additionally applied a combined CO/NOx-isotope model for verification. Here, we separated the CO emissions into different sources based on different CO/NOx emissions ratios for wood combustion and traffic, and inserted this information in the isotope mass balance equation. Accordingly, a highly significant agreement between measured and calculated δ18O-values of CO was found (r=0.67, p<0.001). While different proxies for wood combustion all have their uncertainties, our results indicate that the oxygen isotope ratio of CO (but not the carbon isotope ratio) is an independent sensitive tool for source attribution studies.

Citation: Saurer, M., Prévôt, A. S. H., Dommen, J., Sandradewi, J., Baltensperger, U., and Siegwolf, R. T. W.: The influence of traffic and wood combustion on the stable isotopic composition of carbon monoxide, Atmos. Chem. Phys. Discuss., 8, 19561-19604, doi:10.5194/acpd-8-19561-2008, 2008.
 
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