Firewood residential heating – local versus remote influence on the aerosol burden

Betancourt, Clara; Küppers, Christoph; Piansawan, Tammarat; Sager, Uta; Hoyer, Andrea B.; Kaminski, Heinz; Rapp, Gerhard; John, Astrid C.; Küpper, Miriam; Quass, Ulrich; Kuhlbusch, Thomas; Rudolph, Jochen; Kiendler-Scharr, Astrid; Gensch, Iulia

We report the first-time use of the Lagrangian particle dispersion model (LPDM) FLEXPART to simulate isotope ratios of the biomass burning tracer levoglucosan. Here, we combine the model results with observed levoglucosan concentrations and inline-formulaδ13C to assess the contribution of local vs. remote emissions from firewood domestic heating to the particulate matter sampled during the cold season at two measurements stations of the Environmental Agency of North Rhine-Westphalia, Germany.

For the investigated samples, the simulations indicate that the largest part of the sampled aerosol is 1 to 2 d old and thus originates from local to regional sources. Consequently, ageing, also limited by the reduced photochemical activity in the dark cold season, has a minor influence on the observed levoglucosan concentration and inline-formulaδ13C. The retro plume ages agree well with those derived from observed inline-formulaδ13C (the “isotopic” ages), demonstrating that the limitation of backwards calculations to 7 d for this study does not introduce any significant bias. A linear regression analysis applied to the experimental levoglucosan inline-formulaδ13C vs. the inverse concentration confirms the young age of aerosol. The high variability in the observed inline-formulaδ13C implies that the local levoglucosan emissions are characterized by different isotopic ratios in the range of inline-formula−26.3 ‰ to inline-formula−21.3 ‰. These values are in good agreement with previous studies on levoglucosan source-specific isotopic composition in biomass burning aerosol. Comparison between measured and estimated levoglucosan concentrations suggests that emissions are underestimated by a factor of 2 on average. These findings demonstrate that the aerosol burden from home heating in residential areas is not of remote origin. In this work we show that combining Lagrangian modelling with isotope ratios is valuable to obtain additional insight into source apportionment. Error analysis shows that the largest source of uncertainty is limited information on isotope ratios of levoglucosan emissions. Based on the observed low extent of photochemical processing during the cold season, levoglucosan can be used under similar conditions as a conservative tracer without introducing substantial bias.

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Betancourt, Clara / Küppers, Christoph / Piansawan, Tammarat / et al: Firewood residential heating – local versus remote influence on the aerosol burden. 2021. Copernicus Publications.

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