Late-spring and summertime tropospheric ozone and NO 2 in western Siberia and the Russian Arctic: regional model evaluation and sensitivities

摘要

We use a regional chemistry transport model (Weather Research and Forecasting model coupled with chemistry, WRF-Chem) in conjunction with surface observations of tropospheric ozone and Ozone Monitoring Instrument (OMI) satellite retrievals of tropospheric column NO 2 to evaluate processes controlling the regional distribution of tropospheric ozone over western Siberia for late spring and summer in 2011. This region hosts a range of anthropogenic and natural ozone precursor sources, and it serves as a gateway for near-surface transport of Eurasian pollution to the Arctic. However, there is a severe lack of in situ observations to constrain tropospheric ozone sources and sinks in the region. We show widespread negative bias in WRF-Chem tropospheric column NO 2 when compared to OMI satellite observations from May–August, which is reduced when using ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants) v5a emissions (fractional mean bias (FMB)? = ? ? 0.82 to ? 0.73) compared with the EDGAR (Emissions Database for Global Atmospheric Research)-HTAP (Hemispheric Transport of Air Pollution) v2.2 emissions data (FMB? = ? ? 0.80 to ? 0.70). Despite the large negative bias, the spatial correlations between model and observed NO 2 columns suggest that the spatial pattern of NO x sources in the region is well represented. Scaling transport and energy emissions in the ECLIPSE v5a inventory by a factor of 2 reduces column NO 2 bias (FMB? = ? ? 0.66 to ? 0.35), but with overestimates in some urban regions and little change to a persistent underestimate in background regions. Based on the scaled ECLIPSE v5a emissions, we assess the influence of the two dominant anthropogenic emission sectors (transport and energy) and vegetation fires on surface NO x and ozone over Siberia and the Russian Arctic. Our results suggest regional ozone is more sensitive to anthropogenic emissions, particularly from the transport sector, and the contribution from fire emissions maximises in June and is largely confined to latitudes south of 60 ° ?N. Ozone dry deposition fluxes from the model simulations show that the dominant ozone dry deposition sink in the region is to forest vegetation, averaging 8.0?Tg of ozone per month, peaking at 10.3?Tg of ozone deposition during June. The impact of fires on ozone dry deposition within the domain is small compared to anthropogenic emissions and is negligible north of 60 ° ?N. Overall, our results suggest that surface ozone in the region is controlled by an interplay between seasonality in atmospheric transport patterns, vegetation dry deposition, and a dominance of transport and energy sector emissions.