Nitrate Wet Deposition as a Constraint on NOx Emissions and Impacts on Modeled Secondary Pollutants
Amy Christiansen1 and Toan Vo1
1 University of Missouri - Kansas City, Kansas City, MO
Nitrogen oxides (NOx = NO + NO2) play a critical role in regulating tropospheric chemistry, yet NOx emission estimates are subject to large uncertainties, casting doubt on our ability to accurately model secondary pollutants such as ozone and fine particulate matter (PM2.5). In previous work, we have established the use of nitrate wet deposition (NWD) fluxes as a reliable proxy for NOx emissions and trends. Using NWD observations and the chemical transport model GEOS-Chem, we found evidence of NOx overestimates in emissions inventories over the United States and Europe. Adjusting NOx emissions based on NWD fluxes over Europe improved model representation of surface ozone, reducing overestimates by 12%. In this work, we aim to expand our established method to new areas, seasons, and pollutants. Specifically, we constrain seasonal NOx emissions over the Midwestern United States (MWUS) using the National Atmospheric Deposition Program (NADP) NWD fluxes and GEOS-Chem. GEOS-Chem exhibits large biases in ozone and PM2.5 concentrations on a seasonal basis. Over the MWUS, wintertime PM2.5 and summertime ozone are overestimated by 35% and 52% on average, respectively. A common thread underlying model biases of both pollutants is uncertainty in NOx emissions, which are likely overestimated in this region. Our goal is to constrain seasonal NOx emissions to improve model representation of both ozone and PM2.5. Our preliminary results suggest that reducing summertime NOx emissions in the Community Emissions Data System (CEDS) inventory by 60% reduces model overestimates of summertime ozone by 49% across the MWUS. Reducing wintertime NOx emissions in CEDS by 40% reduces PM2.5 overestimates by 8%. Future work includes exploring additional constraints on ammonia and sulfur dioxide emissions using ammonium and sulfate deposition to further improve representation of modeled PM2.5 and its chemical speciation.