Abstract
Abstract. Atmospheric pollution has many profound effects on human health, ecosystems, and the climate. Of concern are high concentrations and deposition of reactive nitrogen (Nr) species, especially of reduced N (gaseous NH3, particulate NH4+). Atmospheric chemistry and transport models (ACTMs) are crucial to understanding sources and impacts of Nr chemistry and its potential mitigation. Here we undertake the first evaluation of the global version of the EMEP MSC-W ACTM driven by WRF meteorology (1∘×1∘ resolution), with a focus on surface concentrations and wet deposition of N and S species relevant to investigation of atmospheric Nr and secondary inorganic aerosol (SIA). The model–measurement comparison is conducted both spatially and temporally, covering 10 monitoring networks worldwide. Model simulations for 2010 compared use of both HTAP and ECLIPSEE (ECLIPSE annual total with EDGAR monthly profile) emissions inventories; those for 2015 used ECLIPSEE only. Simulations of primary pollutants are somewhat sensitive to the choice of inventory in places where regional differences in primary emissions between the two inventories are apparent (e.g. China) but are much less sensitive for secondary components. For example, the difference in modelled global annual mean surface NH3 concentration using the two 2010 inventories is 18 % (HTAP: 0.26 µg m−3; ECLIPSEE: 0.31 µg m−3) but is only 3.5 % for NH4+ (HTAP: 0.316 µg m−3; ECLIPSEE: 0.305 µg m−3). Comparisons of 2010 and 2015 surface concentrations between the model and measurements demonstrate that the model captures the overall spatial and seasonal variations well for the major inorganic pollutants NH3, NO2, SO2, HNO3, NH4+, NO3-, and SO42- and their wet deposition in East Asia, Southeast Asia, Europe, and North America. The model shows better correlations with annual average measurements for networks in Southeast Asia (mean R for seven species: R7‾=0.73), Europe (R7‾=0.67), and North America (R7‾=0.63) than in East Asia (R5‾=0.35) (data for 2015), which suggests potential issues with the measurements in the latter network. Temporally, both model and measurements agree on higher NH3 concentrations in spring and summer and lower concentrations in winter. The model slightly underestimates annual total precipitation measurements (by 13 %–45 %) but agrees well with the spatial variations in precipitation in all four world regions (0.65–0.94 R range). High correlations between measured and modelled NH4+ precipitation concentrations are also observed in all regions except East Asia. For annual total wet deposition of reduced N, the greatest consistency is in North America (0.75–0.82 R range), followed by Southeast Asia (R=0.68) and Europe (R=0.61). Model–measurement bias varies between species in different networks; for example, bias for NH4+ and NO3- is largest in Europe and North America and smallest in East Asia and Southeast Asia. The greater uniformity in spatial correlations than in biases suggests that the major driver of model–measurement discrepancies (aside from differing spatial representativeness and uncertainties and biases in measurements) are shortcomings in absolute emissions rather than in modelling the atmospheric processes. The comprehensive evaluations presented in this study support the application of this model framework for global analysis of current and potential future budgets and deposition of Nr and SIA.
Highlights
In view of increasing growth in global anthropogenic emissions, the physical and chemical behaviour of reactive nitrogen (Nr) species, especially those that contain reduced N have been explored in both experimental and modelling studies (Liu et al, 2019; Wagner et al, 2020; Ciarelli et al, 2019; Tang et al, 2021)
As the predominant alkaline gas, NH3 exerts significant control on the formation of ambient particles and the acidity of deposition. It readily reacts with H2SO4 and HNO3, and the ammonium sulfate ((NH4)2SO4) and nitrate (NH4NO3) particles formed in these reactions are important in Earth’s radiation budget (Laskin et al, 2015) due to their capacity to act as cloud condensation nuclei and to absorb/scatter solar radiation
Clear differences between the two emission inventories are observed in China, India, and several Southeast Asian countries, but differences in other world regions are relatively small: more than 70 % of the relative differences in ECLIPSEE HTAP emissions, the majority of which are positive, are within ±10 % of the average inventory emission for that grid
Summary
In view of increasing growth in global anthropogenic emissions, the physical and chemical behaviour of reactive nitrogen (Nr) species, especially those that contain reduced N (i.e. gaseous NH3 and particulate NH4+) have been explored in both experimental and modelling studies (Liu et al, 2019; Wagner et al, 2020; Ciarelli et al, 2019; Tang et al, 2021). As the predominant alkaline gas, NH3 exerts significant control on the formation of ambient particles and the acidity of deposition. It readily reacts with H2SO4 and HNO3 (respectively derived from emissions of SO2 and NOx), and the ammonium sulfate ((NH4)2SO4) and nitrate (NH4NO3) particles formed in these reactions are important in Earth’s radiation budget (Laskin et al, 2015) due to their capacity to act as cloud condensation nuclei and to absorb/scatter solar radiation. Excessive anthropogenic reduced N emissions to the atmosphere can lead to severe eutrophication and formation of hypoxic zones, with their consequent threats to ecosystem diversity (Erisman et al, 2005)
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