Quantifying international and interstate contributions to primary ambient PM2.5 and PM10 in a complex metropolitan atmosphere

Abstract

We quantify the contributions of long-range and regionally transported aerosols to ambient primary PM2.5 and PM10 in a representative United States industrialized/urban atmosphere via detailed elemental analysis and chemical mass balance (CMB) modeling after identifying their presence using a variety of publicly available satellite data/information, software products, and synoptic-scale aerosol models. A year-long study in Houston, Texas identified North African dust as the principal long-range global source of primary particulate matter (PM). CMB estimated transatlantic dust from the Sahara-Sahel region to be dominant in the summer months contributing an average of 3.5 μg m−3 to PM2.5 and 7.9 μg m−3 to PM10 during May–August, i.e., the active Saharan dust season. Biomass burning was the chief source of regionally transported PM impacting air quality on different occasions throughout the year depending on the fire location. Four major biomass combustion events affecting air quality in Texas were calculated to contribute an average of 1.3 μg m−3 to PM2.5 and 1.4 μg m−3 to PM10 in corresponding samples whose origins were tracked to Canada, southeastern states of USA, and Central America using fire maps, HYSPLIT back trajectories, and the Navy Aerosol Analysis and Prediction System global aerosol model. Elemental concentrations and signature ratios revealed significant mixing of potassium, rare earth metals, and vanadium from proximal and distal crustal (natural) sources with anthropogenically emitted PM. This demonstrates the need to isolate the non-mineral components of these metals to employ them as tracers for primary PM emitted by biomass burning, petroleum refineries, and oil combustion. Transboundary contributions to primary PM2.5 were 1.5 μg m−3 and 3.1 μg m−3 to PM10 adding 16% to annual average mass concentration of both size fractions demonstrating that local sources were primarily responsible for ambient air quality with non-trivial contributions from international and interstate sources. Rigorously identifying and quantifying aerosol sources assists in improving air quality management policies designed to protect public health and comply with ever-decreasing federal PM standards that allow state agencies to exclude contributions that are not reasonably controllable or preventable from regulatory decisions and actions.