The impacts of regional shipping emissions on the chemical characteristics of coastal submicron aerosols near Houston, TX

Abstract

The air quality of the Texas Gulf Coast region historically has been influenced heavily by regional shipping emissions. However, the effects of the recently established North American Emissions Control Area on aerosol concentrations and properties in this region are presently unknown. In order to better understand the current sources and processing mechanisms influencing coastal aerosol near Houston, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed for 3 weeks at a coastal location during May–June 2016. Total mass loadings of organic and inorganic non-refractory aerosol components during onshore flow periods were similar to those published before establishment of the regulations. Based on estimated methanesulfonic acid (MSA) mass loadings and published biogenic MSA / non-sea-salt sulfate (nss-SO4) ratios, an average of over 75 % of the observed nss-SO4 was from anthropogenic sources, predominantly shipping emissions. Mass spectral analysis indicated that for periods with similar backward-trajectory-averaged meteorological conditions, air masses influenced by shipping emissions had an increased mass fraction of ions related to carboxylic acids and larger oxygen-to-carbon ratios than those that avoided shipping lanes, suggesting that shipping emissions increase marine organic aerosol (OA) oxidation state. Amine fragment mass loadings were correlated positively with anthropogenic nss-SO4 during onshore flow, implying anthropogenic–biogenic interaction in marine OA production. Model calculations also suggest that advection of shipping-derived aerosol may enhance inland aqueous-phase secondary OA production. These results imply a continuing role of shipping emissions on aerosol properties over the Gulf of Mexico and suggest that further regulation of shipping fuel sulfur content will reduce coastal submicron aerosol mass loadings near Houston.