Evaluating NO_<i>x</i> stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO₂ columns

Abstract

This paper presents large-eddy simulations with atmospheric chemistry of four large point sources world-wide, focusing on the evaluation of NOx (NO + NO2) emissions with the TROPOspheric Monitoring Instrument (TROPOMI). We implemented a condensed chemistry scheme to investigate how the emitted NOx (95 % as NO) is converted to NO2 in the plume. To use NOx as a proxy for CO2 emission, information about its atmospheric lifetime and the fraction of NOx present as NO2 is required. We find that the chemical evolution of the plumes depends strongly on the amount of NOx that is emitted, as well as on wind speed and direction. For large NOx emissions, the chemistry is pushed in a high-NOx chemical regime over a length of almost 100 km downwind of the stack location. Other plumes with lower NOx emissions show a fast transition to an intermediate-NOx chemical regime, with short NOx lifetimes. Simulated NO2 columns mostly agree within 20 % with TROPOMI, signalling that the emissions used in the model were approximately correct. However, variability in the simulations is large, making a one-to-one comparison difficult. We find that temporal wind speed variations should be accounted for in emission estimation methods. Moreover, results indicate that common assumptions about the NO2 lifetime (≈ 4 h) and NOx:NO2 ratios (≈ 1.3) in simplified methods that estimate emissions from NO2 satellite data need revision.