Abstract

Abstract. Energy security and climate change concerns have led to the promotion of biomass-derived ethanol, an oxygenated volatile organic compound (OVOC), as a substitute for fossil fuels. Although ethanol is ubiquitous in the troposphere, our knowledge of its current atmospheric budget and distribution is limited. Here, for the first time we use a global chemical transport model in conjunction with atmospheric observations to place constraints on the ethanol budget, noting that additional measurements of ethanol (and its precursors) are still needed to enhance confidence in our estimated budget. Global sources of ethanol in the model include 5.0 Tg yr−1 from industrial sources and biofuels, 9.2 Tg yr−1 from terrestrial plants, ~0.5 Tg yr−1 from biomass burning, and 0.05 Tg yr−1 from atmospheric reactions of the ethyl peroxy radical (C2H5O2) with itself and with the methyl peroxy radical (CH3O2). The resulting atmospheric lifetime of ethanol in the model is 2.8 days. Gas-phase oxidation by the hydroxyl radical (OH) is the primary global sink of ethanol in the model (65%), followed by dry deposition (25%), and wet deposition (10%). Over continental areas, ethanol concentrations predominantly reflect direct anthropogenic and biogenic emission sources. Uncertainty in the biogenic ethanol emissions, estimated at a factor of three, may contribute to the 50% model underestimate of observations in the North American boundary layer. Current levels of ethanol measured in remote regions are an order of magnitude larger than those in the model, suggesting a major gap in understanding. Stronger constraints on the budget and distribution of ethanol and OVOCs are a critical step towards assessing the impacts of increasing the use of ethanol as a fuel.

Highlights

  • The use of bio-ethanol is currently being promoted as a renewable fuel that will alleviate dependence on fossil fuels and combat global warming

  • Naik et al.: Observational constraints on global atmospheric budget of ethanol

  • Similar to the previous source estimate, biogenic emissions account for the largest fraction of emissions (63%) in our inventory; we estimate a larger contribution from anthropogenic sources including biofuels (33%), and smaller contributions from biomass burning (3%) and atmospheric production (

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Summary

Introduction

The use of bio-ethanol (ethanol derived from biomass) is currently being promoted as a renewable fuel that will alleviate dependence on fossil fuels and combat global warming. Measurements off the coast of New England in July–August 2002 suggest that the ethanol source is largely anthropogenic with a small biogenic source but no discernible secondary source from atmospheric production (de Gouw et al, 2005) These studies highlight regional variations in ethanol sources, making it difficult to determine the global budget solely from the limited set of available observations. A previous simulation using MOZART-4 with a similar configuration was evaluated with aircraft measurements of ozone and its precursors over the northeastern United States in summer 2004 during the Intercontinental Chemical Transport Experiment – North America (INTEX-NA) and was found to resolve boundary layer ventilation as indicated by the model skill at capturing the observed campaign-mean vertical profiles of carbon monoxide, ethane, and other hydrocarbons (Horowitz et al, 2007)

Ethanol sources
Ethanol sinks
Results and discussion
Conclusions
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