Evaluation of nitrogen oxides (NOx) sources and sinks and ozone production in Colombia and surrounding areas

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Abstract

In Colombia, industrialization and a shift towards intensified agriculture have led to increased emissions of air pollutants. However, the baseline state of air quality in Colombia is relatively unknown. In this study we aim to assess the baseline state of air quality in Colombia with a focus on the spatial and temporal variability in emissions and atmospheric burden of nitrogen oxides (NOx = NO + NO2) and evaluate surface NOx , ozone (O3) and carbon monoxide (CO) mixing ratios. We quantify the magnitude and spatial distribution of the four major NOx sources (lightning, anthropogenic activities, soil biogenic emissions and biomass burning) by integrating global NOx emission inventories into the mesoscale meteorology and atmospheric chemistry model, namely Weather Research and Forecasting (WRF) coupled with Chemistry (collectively WRF-Chem), at a similar resolution ( 25 km) to the Emission Database for Global Atmospheric Research (EDGAR) anthropogenic emission inventory and the Ozone Monitoring Instrument (OMI) remote sensing observations. The model indicates the largest contribution by lightning emissions (1258 GgNyr1), even after already significantly reducing the emissions, followed by anthropogenic (933 GgNyr1), soil biogenic (187 GgNyr1) and biomass burning emissions (104 GgNyr1). The comparison with OMI remote sensing observations indicated a mean bias of tropospheric NO2 columns over the whole domain (WRF-Chem minus OMI) of 0.02 (90% CI: [0:43, 0.70])1015 molecules cm2, which is < 5% of the mean column. However, the simulated NO2 columns are overestimated and underestimated in regions where lightning and biomass burning emissions dominate, respectively. WRFChem was unable to capture NOx and CO urban pollutant mixing ratios, neither in timing nor in magnitude. Yet, WRFChem was able to simulate the urban diurnal cycle of O3 satisfactorily but with a systematic overestimation of 10 parts per billion (ppb) due to the equally large underestimation of NO mixing ratios and, consequently, titration. This indicates that these city environments are in the NOx-saturated regime with frequent O3 titration. We conducted sensitivity experiments with an online meteorology-chemistry singlecolumn model (SCM) to evaluate how WRF-Chem subgridscale- enhanced emissions could explain an improved representation of the observed O3, CO and NOx diurnal cycles. Interestingly, the SCM simulation, showing especially a shallower nocturnal inversion layer, results in a better representation of the observed diurnal cycle of urban pollutant mixing ratios without an enhancement in emissions. This stresses that, besides application of higher-resolution emission inventories and model experiments, the diurnal cycle in boundary layer dynamics (and advection) should be critically evaluated in models such as WRF-Chem to assess urban air quality. Overall, we present a concise method to quantify air quality in regions with limited surface measurements by integrating in situ and remote sensing observations. This study identifies four distinctly different source regions and shows their interannual and seasonal variability during the last 1.5 decades. It serves as a base to assess scenarios of future air quality in Colombia or similar regions with contrasting emission regimes, complex terrain and a limited air quality monitoring network.

Original languageEnglish
Pages (from-to)9441-9458
Number of pages18
JournalAtmospheric Chemistry and Physics
Volume20
Issue number15
DOIs
Publication statusPublished - 12 Aug 2020

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