Emissions of nitrogen oxides from US urban areas: estimation from Ozone Monitoring Instrument retrievals for 2005-2014
Satellite remote sensing of tropospheric nitrogen dioxide (NO 2 ) can provide valuable information for estimating surface nitrogen oxides (NO x ) emissions. Using an exponentially-modified Gaussian (EMG) method and taking into account the effect of wind on observed NO 2 distributions, we estimate three-year moving-average emissions of summertime NO x from 35 US urban areas directly from NO 2 retrievals of the Ozone Monitoring Instrument (OMI) during 2005–2014. Following the conclusions of previous studies that the EMG method provides robust and accurate emission estimates under strong-wind conditions, we derive top-down NO x emissions from each urban area by applying the EMG method to OMI data with wind speeds greater than 3–5 m s -1 . Meanwhile, we find that OMI NO 2 observations under weak-wind conditions (i.e., < 3 m s -1 ) are qualitatively better correlated with the surface NO x source strength in comparison to all-wind OMI maps; and therefore we use them to calculate the satellite-observed NO 2 burdens of urban areas and compare with NO x emission estimates. The EMG results show that OMI-derived NO x emissions are highly correlated ( R > 0.93) with weak-wind OMI NO 2 burdens as well as bottom-up NO x emission estimates over 35 urban areas, implying a linear response of the OMI observations to surface emissions under weak-wind conditions. The simultaneous, EMG-obtained, effective NO 2 lifetimes (~3.5 ± 1.3 h), however, are biased low in comparison to the summertime NO 2 chemical lifetimes. In general, isolated urban areas with NO x emission intensities greater than ~ 2 Mg h -1 produce statistically significant weak-wind signals in three-year average OMI data. From 2005 to 2014, we estimate that total OMI-derived NO x emissions over all selected US urban areas decreased by 49%, consistent with reductions of 43, 47, 49, and 44% in the total bottom-up NO x emissions, the sum of weak-wind OMI NO 2 columns, the total weak-wind OMI NO 2 burdens, and the averaged NO 2 concentrations, respectively, reflecting the success of NO x control programs for both mobile sources and power plants. The decrease rates of these NO x -related quantities are found to be faster (i.e., -6.8 to -9.3% yr -1 ) before 2010 and slower (i.e., -3.4 to -4.9% yr -1 ) after 2010. For individual urban areas, we calculate the R values of pair-wise trends among the OMI-derived and bottom-up NO x emissions, the weak-wind OMI NO 2 burdens, and ground-based NO 2 measurements; and high correlations are found for all urban areas (median R = 0.8), particularly large ones ( R up to 0.97). The results of the current work indicate that using the EMG method and considering the wind effect, the OMI data allow for the estimation of NO x emissions from urban areas and the direct constraint of emission trends with reasonable accuracy.