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Title: 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 overmore » 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.« less
Authors:
 [1] ;  [1] ; ORCiD logo [2] ;  [3] ;  [4] ;  [5]
  1. Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Saint Louis Univ., St. Louis, MO (United States)
  3. Goddard Earth Sciences Technology and Research, Universities Space Research Association, Columbia, MD (United States); NASA Goddard Space Flight Center, Greenbelt, MD (United States)
  4. NASA Goddard Space Flight Center, Greenbelt, MD (United States)
  5. US Environmental Protection Agency, Research Triangle Park, NC (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Atmospheric Chemistry and Physics Discussions (Online)
Additional Journal Information:
Journal Name: Atmospheric Chemistry and Physics Discussions (Online); Journal Volume: 15; Journal Issue: 10; Journal ID: ISSN 1680-7375
Publisher:
European Geosciences Union
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES
OSTI Identifier:
1208944