Joint analysis of deposition fluxes and atmospheric concentrations of inorganic nitrogen and sulphur compounds predicted by six chemistry transport models in the frame of the EURODELTAIII project

Abstract

In the framework of the UNECE Task Force on Measurement and Modelling (TFMM) under the Convention on Long-range Transboundary Air Pollution (LRTAP), the EURODELTAIII project is evaluating how well air quality models are able to reproduce observed pollutant air concentrations and deposition fluxes in Europe. In this paper the sulphur and nitrogen deposition estimates of six state-of-the-art regional models (CAMx, CHIMERE, EMEP MSC-W, LOTOS-EUROS, MINNI and CMAQ) are evaluated and compared for four intensive EMEP measurement periods (25 Feb - 26 Mar 2009; 17 Sep - 15 Oct 2008; 8 Jan – 4 Feb 2007 and 1–30 Jun 2006). For sulphur, this study shows the importance of including sea salt sulphate emissions for obtaining better model results; CMAQ, the only model considering these emissions in its formulation, was the only model able to reproduce the high measured values of wet deposition of sulphur at coastal sites. MINNI and LOTOS-EUROS underestimate sulphate wet deposition for all periods and have low wet deposition efficiency for sulphur. For reduced nitrogen, all the models underestimate both wet deposition and total air concentrations (ammonia plus ammonium) in the summer campaign, highlighting a potential lack of emissions (or incoming fluxes) in this period. In the rest of campaigns there is a general underestimation of wet deposition by all models (MINNI and CMAQ with the highest negative bias), with the exception of EMEP, which underestimates the least and even overestimates deposition in two campaigns. This model has higher scavenging deposition efficiency for the aerosol component, which seems to partly explain the different behaviour of the models. For oxidized nitrogen, CMAQ, CAMx and MINNI predict the lowest wet deposition and the highest total air concentrations (nitric acid plus nitrates). Comparison with observations indicates a general underestimation of wet oxidized nitrogen deposition by these models, as well as an overestimation of total air concentration for all the campaigns, except for the 2006 campaign. This points to a low efficiency in the wet deposition of oxidized nitrogen for these models, especially with regards to the scavenging of nitric acid, which is the main driver of oxidized N deposition for all the models. CHIMERE, LOTOS-EUROS and EMEP agree better with the observations for both wet deposition and air concentration of oxidized nitrogen, although CHIMERE seems to overestimate wet deposition in the summer period. This requires further investigation, as the gas-particle equilibrium seems to be biased towards the gas phase (nitric acid) for this model. In the case of MINNI, the frequent underestimation of wet deposition combined with an overestimation of atmospheric concentrations for the three pollutants indicates a low efficiency of the wet deposition processes. This can be due to several reasons, such as an underestimation of scavenging ratios, large vertical concentration gradients (resulting in small concentrations at cloud height) or a poor parameterization of clouds. Large differences between models were also found for the estimates of dry deposition. However, the lack of suitable measurements makes it impossible to assess model performance for this process. These uncertainties should be addressed in future research, since dry deposition contributes significantly to the total deposition for the three deposited species, with values in the same range as wet deposition for most of the models, and with even higher values for some of them, especially for reduced nitrogen.