We present a new method to infer nitrogen oxides (NOx) emissions and lifetimes based on tropospheric nitrogen dioxide (NO2) observations together with reanalysis wind fields for cities located in polluted backgrounds. Since the accuracy of the method is difficult to assess due to lack of “true values” that can be used as a benchmark, we apply the method to synthetic NO2 observations derived from a high-resolution model simulation for cities over the continental US and compare the inferred emissions and lifetimes with the values given by the model to evaluate the method. The method is applicable to 26 US cities. The derived results are generally in good agreement with the values given by the model, with the relative differences of 2?% ± 17?% (mean ± standard deviation) and 15?% ± 25?% for lifetimes and emissions, respectively. Our investigation suggests that the use of wind data prior to satellite overpass time improves the performance of the method. The correlation coefficients between inferred and NU-WRF lifetimes increase from 0.56 to 0.79 and for emissions increase from 0.88 to 0.96 when comparing results based on wind fields sampled simultaneously with satellite observations and averaged over 9 hours data prior to satellite observations, respectively. We estimate that uncertainties in NOx lifetime and emissions arising from the method are approximately 15 % and 20 %, respectively, for typical (US) cities. We expect this new method to be applicable to NO2 observations from the TROPOspheric Monitoring Instrument (TROPOMI) and geostationary satellites, such as Geostationary Environment Monitoring Spectrometer (GEMS) or the Tropospheric Emissions: Monitoring Pollution (TEMPO) instrument, to estimate urban NOx emissions and lifetimes globally.
Published: February 25, 2022
Citation
Liu F., Z. Tao, S. Beirle, J. Joiner, Y. Yoshida, S.J. Smith, and K.E. Knowland, et al. 2022.A new method for inferring city emissions and lifetimes of nitrogen oxides from high-resolution nitrogen dioxide observations: A model study.Atmospheric Chemistry and Physics 22, no. 2:1333-1349.PNNL-SA-166725.doi:10.5194/acp-22-1333-2022