Low modeled ozone production suggests underestimation of precursor emissions (especially NO_<i>x</i>) in Europe

Emmanouil Oikonomakis , Sebnem Aksoyoglu (1) , Giancarlo Ciarelli (1, 2, 3) , Urs Baltensperger (4) , André Stephan Henry Prévôt (4)

1 LAC - Laboratory of Atmospheric Chemistry [Paul Scherrer Institute]
2 LISA (UMR_7583) - Laboratoire Interuniversitaire des Systèmes Atmosphériques
3 LISA (UMR_7583) - Laboratoire Interuniversitaire des Systèmes Atmosphériques
4 PSI - Paul Scherrer Institute

Abstract. High surface ozone concentrations, which usually occur when photochemical ozone production takes place, pose a great risk to human health and vegetation. Air quality models are often used by policy makers as tools for the development of ozone mitigation strategies. However, the modeled ozone production is often not or not enough evaluated in many ozone modeling studies. The focus of this work is to evaluate the modeled ozone production in Europe indirectly, with the use of the ozone–temperature correlation for the summer of 2010 and to analyze its sensitivity to precursor emissions and meteorology by using the regional air quality model, the Comprehensive Air Quality Model with Extensions (CAMx). The results show that the model significantly underestimates the observed high afternoon surface ozone mixing ratios (≥ 60 ppb) by 10–20 ppb and overestimates the lower ones (< 40 ppb) by 5–15 ppb, resulting in a misleading good agreement with the observations for average ozone. The model also underestimates the ozone–temperature regression slope by about a factor of 2 for most of the measurement stations. To investigate the impact of emissions, four scenarios were tested: (i) increased volatile organic compound (VOC) emissions by a factor of 1.5 and 2 for the anthropogenic and biogenic VOC emissions, respectively, (ii) increased nitrogen oxide (NOx) emissions by a factor of 2, (iii) a combination of the first two scenarios and (iv) increased traffic-only NOx emissions by a factor of 4. For southern, eastern, and central (except the Benelux area) Europe, doubling NOx emissions seems to be the most efficient scenario to reduce the underestimation of the observed high ozone mixing ratios without significant degradation of the model performance for the lower ozone mixing ratios. The model performance for ozone–temperature correlation is also better when NOx emissions are doubled. In the Benelux area, however, the third scenario (where both NOx and VOC emissions are increased) leads to a better model performance. Although increasing only the traffic NOx emissions by a factor of 4 gave very similar results to the doubling of all NOx emissions, the first scenario is more consistent with the uncertainties reported by other studies than the latter, suggesting that high uncertainties in NOx emissions might originate mainly from the road-transport sector rather than from other sectors. The impact of meteorology was examined with three sensitivity tests: (i) increased surface temperature by 4 ∘C, (ii) reduced wind speed by 50 % and (iii) doubled wind speed. The first two scenarios led to a consistent increase in all surface ozone mixing ratios, thus improving the model performance for the high ozone values but significantly degrading it for the low ozone values, while the third scenario had exactly the opposite effects. Overall, the modeled ozone is predicted to be more sensitive to its precursor emissions (especially traffic NOx) and therefore their uncertainties, which seem to be responsible for the model underestimation of the observed high ozone mixing ratios and ozone production.

Domaines: Sciences de l'environnement

Emmanouil Oikonomakis, Sebnem Aksoyoglu, Giancarlo Ciarelli, Urs Baltensperger, André Stephan Henry Prévôt. Low modeled ozone production suggests underestimation of precursor emissions (especially NO_<i>x</i>) in Europe. Atmospheric Chemistry and Physics, 2018, 18 (3), pp.2175-2198. ⟨10.5194/acp-18-2175-2018⟩. ⟨hal-04568592⟩