Using satellite observations of tropospheric NO2 columns to infer long-term trends in US NOx emissions: the importance of accounting for the free tropospheric NO2 background

摘要

The National Emission Inventory (NEI) of the US Environmental Protection Agency (EPA) reports a steady decrease in US NOx emissions over the 2005-2017 period at a rate of 0.1 Tg N a(-1) (53 % decrease over the period), reflecting sustained efforts to improve air quality. Tropospheric NO2 columns observed by the satellite-based Ozone Monitoring Instrument (OMI) over the US show a steady decrease until 2009 but a flattening afterward, which has been attributed to a flattening of NOx emissions, contradicting the NEI. We show here that the steady 2005-2017 decrease in NOx emissions reported by the NEI is in fact largely consistent with observed network trends of surface NO2 and ozone concentrations. The OMI NO2 trend is instead similar to that observed for nitrate wet deposition fluxes, which is weaker than that for anthropogenic NOx emissions, due to a large and increasing relative contribution of non-anthropogenic background sources of NOx (mainly lightning and soils). This is confirmed by contrasting OMI NO2 trends in urban winter, where the background is low and OMI NO2 shows a 2005-2017 decrease consistent with the NEI, and rural summer, where the background is high and OMI NO2 shows no significant 2005-2017 trend. A GEOS -Chem model simulation driven by NEI emission trends for the 2005-2017 period reproduces these different trends, except for the post-2009 flattening of OMI NO2, which we attribute to a model underestimate of free tropospheric NO2. Better understanding is needed of the factors controlling free tropospheric NO2 in order to relate satellite observations of tropospheric NO2 columns to the underlying NOx emissions and their trends. Focusing on urban winter conditions in the satellite data minimizes the effect of this free tropospheric background.