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Emissions of C-6-C-8 aromatic compounds in the United States: Constraints from tall tower and aircraft measurements
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2015
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Source: Journal of Geophysical Research-Atmospheres, 120(2), 826-842.
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Journal Title:Journal of Geophysical Research: Atmospheres
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Description:We present two full years of continuous C-6-C-8 aromatic compound measurements by PTR-MS at the KCMP tall tower (Minnesota, US) and employ GEOS-Chem nested grid simulations in a Bayesian inversion to interpret the data in terms of new constraints on US aromatic emissions. Based on the tall tower data, we find that the RETRO inventory (year-2000) overestimates US C-6-C-8 aromatic emissions by factors of 2.0-4.5 during 2010-2011, likely due in part to post-2000 reductions. Likewise, our implementation of the US EPA's NEI08 overestimates the toluene flux by threefold, reflecting an inventory bias in non-road emissions plus uncertainties associated with species lumping. Our annual top-down emission estimates for benzene and C-8 aromatics agree with the NEI08 bottom-up values, as does the inferred contribution from non-road sources. However, the NEI08 appears to underestimate on-road emissions of these compounds by twofold during the warm season. The implied aromatic sources upwind of North America are more than double the prior estimates, suggesting a substantial underestimate of East Asian emissions, or large increases there since 2000. Long-range transport exerts an important influence on ambient benzene over the US: on average 43% of its wintertime abundance in the US Upper Midwest is due to sources outside North America. Independent aircraft measurements show that the inventory biases found here for C-6-C-8 aromatics also apply to other parts of the US, with notable exceptions for toluene in California and Houston, Texas. Our best estimates of year-2011 contiguous US emissions are 206 (benzene), 408 (toluene), and 822 (C-8 aromatics) GgC.
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Source:Journal of Geophysical Research-Atmospheres, 120(2), 826-842.
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