Improvement of the satellite-derived NOix/i emissions on air quality modeling and its effect on ozone and secondary inorganic aerosol formation in the Yangtze River Delta, China

Abstract

We developed a top-down methodology combining the inversed chemistry transport modeling and satellitederived tropospheric vertical column of NO2 and estimated the NOx emissions of the Yangtze River Delta (YRD) region at a horizontal resolution of 9 km for January, April, July, and October 2016. The effect of the top-down emission estimation on air quality modeling and the response of ambient ozone (O3) and inorganic aerosols (SO24 , NO3 , and NHC 4 , SNA) to the changed precursor emissions were evaluated with the Community Multi-scale Air Quality (CMAQ) system. The top-down estimates of NOx emissions were smaller than those (i.e., the bottom-up estimates) in a national emission inventory, Multi-resolution Emission Inventory for China (MEIC), for all the 4 months, and the monthly mean was calculated to be 260.0 Gg/month, 24% less than the bottom-up one. The NO2 concentrations simulated with the bottom-up estimate of NOx emissions were clearly higher than the ground observations, indicating the possible overestimation in the current emission inventory, attributed to its insufficient consideration of recent emission control in the region. The model performance based on top-down estimate was much better, and the biggest change was found for July, with the normalized mean bias (NMB) and normalized mean error (NME) reduced from 111% to 0.4% and from 111% to 33 %, respectively. The results demonstrate the improvement of NOx emission estimation with the nonlinear inversed modeling and satellite observation constraint. With the smaller NOx emissions in the top-down estimate than the bottom-up one, the elevated concentrations of ambient O3 were simulated for most of the YRD, and they were closer to observations except for July, implying the VOC (volatile organic compound)-limited regime of O3 formation.With available ground observations of SNA in the YRD, moreover, better model performance of NO3 and NHC 4 was achieved for most seasons, implying the effectiveness of precursor emission estimation on the simulation of secondary inorganic aerosols. Through the sensitivity analysis of O3 formation for April 2016, the decreased O3 concentrations were found for most of the YRD region when only VOC emissions were reduced or the reduced rate of VOC emissions was 2 times of that of NOx , implying the crucial role of VOC control in O3 pollution abatement. The SNA level for January 2016 was simulated to decline 12% when 30% of NH3 emissions were reduced, while the change was much smaller with the same reduced rate for SO2 or NOx . The result suggests that reducing NH3 emissions was the most effective way to alleviate SNA pollution of the YRD in winter.