Coupling Sr–Nd–Hf Isotope Ratios and Elemental Analysis to Accurately Quantify North African Dust Contributions to PM2.5 in a Complex Urban Atmosphere by Reducing Mineral Dust Collinearity

Tracking Saharan–Sahelian dust across the globe is essential to elucidate its effects on Earth’s climate, radiation budget, hydrologic cycle, nutrient cycling, and also human health when it seasonally enters populated/industrialized regions of Africa, Europe, and North America. However, the elemental composition of mineral dust arising locally from construction activities and aeolian soil resuspension overlaps with African dust. Therefore, we derived a novel “isotope-resolved chemical mass balance” (IRCMB) method by employing radiogenic strontium, neodymium, and hafnium isotopes to accurately differentiate and quantitatively apportion collinear proximal and synoptic-scale crustal and anthropogenic mineral dust sources. IRCMB was applied to two air masses that transported African dust to Barbados and Texas to track particulate matter (PM) spikes at both locations. During Saharan–Sahelian intrusions, the radiogenic content of urban PM(2.5) increased with respect to (87)Sr/(86)Sr and (176)Hf/(177)Hf but decreased in terms of (143)Nd/(144)Nd, demonstrating the ability of these isotopes to sensitively track African dust intrusions even in complex metropolitan atmospheres. The principal aerosol strontium, neodymium, and hafnium end members were concrete dust and soil, soil and motor vehicles, and motor vehicles and North African dust, respectively. IRCMB separated and quantified local soil and distal crustal dust even when PM(2.5) concentrations were low, opening a promising source apportionment avenue for urbanized/industrialized atmospheres.