Impact of mineral dust on nitrate, sulfate, and ozone in transpacific Asian pollution plumes

摘要

We use a 3-D global chemical transport model (GEOS-Chem) to interpret aircraft observations of nitrate and sulfate partitioning in transpacific dust plumes during the INTEX-B campaign of April-May 2006. The model includes explicit transport of size-resolved mineral dust and its alkalinity, nitrate, and sulfate content. The observations show that particulate nitrate is primarily associated with dust, sulfate is primarily associated with ammonium, and Asian dust remains alkaline across the Pacific. This can be reproduced in the model by using a reactive uptake coefficient for HNO3 on dust (gamma(HNO3) similar to 10(-3)) much lower than commonly assumed in models and possibly reflecting limitation of uptake by dust dissolution. The model overestimates gas-phase HNO3 by a factor of 2-3, typical of previous model studies; we show that this cannot be corrected by uptake on dust. We find that the fraction of aerosol nitrate on dust in the model increases from similar to 30% in fresh Asian outflow to 80-90% over the Northeast Pacific, reflecting in part the volatilization of ammonium nitrate and the resulting transfer of nitrate to the dust. Consumption of dust alkalinity by uptake of acid gases in the model is slow relative to the lifetime of dust against deposition, so that dust does not acidify (at least not in the bulk). This limits the potential for dust iron released by acidification to become bio-available upon dust deposition. Observations in INTEX-B show no detectable ozone depletion in Asian dust plumes, consistent with the model. Uptake of HNO3 by dust, suppressing its recycling to NOx, reduces Asian pollution influence on US surface ozone in the model by 10-15% or up to 1 ppb.