Satellite constraint for emissions of nitrogen oxides from anthropogenic, lightning and soil sources over East China on a high-resolution grid

Abstract

Abstract. Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from space provide valuable information to estimate emissions of nitrogen oxides (NOx) inversely. Accurate emission attribution to individual sources, important both for understanding the global biogeochemical cycling of nitrogen and for emission control, remains difficult. This study presents a regression-based multi-step inversion approach to estimate emissions of NOx from anthropogenic, lightning and soil sources individually for 2006 over East China on a 0.25° long × 0.25° lat grid, employing the DOMINO product version 2 retrieved from the Ozone Monitoring Instrument. The inversion is done gridbox by gridbox to derive the respective emissions, taking advantage of differences in seasonality between anthropogenic and natural sources. Lightning and soil emissions are combined together for any given gridbox due to their similar seasonality; and their different spatial distributions are used implicitly for source separation to some extent. The nested GEOS-Chem model for East Asia is used to simulate the seasonal variations of different emission sources and impacts on VCDs of NO2 for the inversion purpose. Sensitivity tests are conducted to evaluate key assumptions embedded in the inversion process. The inverse estimate suggests annual budgets of about 7.1 TgN (±39%), 0.21 TgN (±61%), and 0.38 TgN (±65%) for the a posteriori anthropogenic, lightning and soil emissions, respectively, about 18–23% higher than the respective a priori values. The enhancements in anthropogenic emissions are largest in cities and areas with extensive use of coal, particularly in the north in winter, as evident on the high-resolution grid. Derived soil emissions are consistent with recent bottom-up estimates. They are less than 6% of anthropogenic emissions annually, increasing to about 13% for July. Derived lightning emissions are about 3% of anthropogenic emissions annually and about 10% in July. Overall, anthropogenic emissions are found to be the dominant source of NOx over East China with important implications for nitrogen control.