Abstract

Observational constraints to biomass burning (BB) NOx emissions as provided by satellite measurements of nitrogen dioxide (NO2) critically depend on quantitative assumptions regarding the atmospheric NOx lifetime. In this study, we investigated NOx emissions from the extreme wildfires that occurred in the European part of Russia in summer 2010 by using an original inverse modeling method that allowed us to avoid any a priori assumptions regarding the NOx lifetime. The method was applied to the tropospheric NO2 columns retrieved from the measurements performed by the OMI satellite instrument, while the relationship between BB NOx emissions and tropospheric NO2 columns was simulated with the CHIMERE mesoscale chemistry transport model. Our analysis indicated that this relationship depends strongly on BB emissions of volatile organic compounds and that a dependence of the effective NOx lifetime on the NOx fluxes can be essentially nonlinear. Our estimates of the total NOx emissions in the study region are found to be at least 40% larger compared to the respective data from the GFASv1.0 and GFED4.1s global fire emission inventories.

Highlights

  • Nitrogen oxides (NOx = NO + NO2 ) are important atmospheric constituents affecting climate processes and air quality by serving as precursors of tropospheric ozone [1,2] and influencing secondary aerosol formation [3,4]

  • biomass burning (BB) NOx emissions can play a predominant role in the oxidation processes leading to ozone formation inside smoke plumes from wildfires [6] over other NOx sources and provide a major contribution to NO2 column amounts over fire spots [7]

  • Available BB NOx emission estimates provided by fire emission inventories (e.g., [8,9]) based on indirect measurements of the amounts of biomass burned have mostly not been validated against atmospheric measurements and are likely to be rather uncertain as indicated by a diversity of the

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Summary

Introduction

One of the significant sources of NOx on a global scale is associated with open biomass burning (BB): it is estimated that BB provides around 15% of total NOx emissions globally [5]. BB NOx emissions can play a predominant role in the oxidation processes leading to ozone formation inside smoke plumes from wildfires [6] over other NOx sources and provide a major contribution to NO2 column amounts over fire spots [7]. Despite the important role played by BB NOx emissions in atmospheric processes, the current knowledge of the amounts of NOx emitted into the atmosphere from wildfires is insufficient. Validation of BB NOx emission estimates is more difficult compared to validation of BB emissions of some other species (such as, e.g., CO) due to high reactivity and a Atmosphere 2016, 7, 132; doi:10.3390/atmos7100132 www.mdpi.com/journal/atmosphere

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