Seasonal variation of atmospheric Pb sources in Singapore - Elemental and lead isotopic compositions of PM10 as source tracer

Abstract

Southeast Asia has become a hotspot of anthropogenic particulate matter (PM) emissions due to increased coal combustion, high-temperature industrial operations, vehicular traffic, and agricultural biomass burning. Lead (Pb), a criteria pollutant, bound to such PM can be hazardous when inhaled, even at extremely low concentrations. Precise and accurate source apportionment of atmospheric Pb is thus, critical in order to minimize its exposure. This study investigates the sources of atmospheric Pb in Singapore aerosol samples (PM10) using Pb isotopes and elemental composition as tracers of contamination sources. PM10 aerosol sampling was conducted over a period of 1 year from June 2017 to May 2018 to capture the seasonal variations in sources of atmospheric Pb. Elemental concentrations reveal particularly high enrichment factors for Pb, Cu, V, Ni and Zn, especially when under the influence of southwest (SW) and inter monsoon (IM) winds. Pb isotopic ratios across the three seasons (206/207Pb = 1.147˗1.150 and 208/207Pb = 2.420˗2.428) are not significantly different. The Pb isotopic signatures and V/Ni ratios for all three seasons overlap with those of gasoline, diesel and ship emissions. Moreover, V/Pb values of more than unity for SW and IM winds suggest influence of transboundary coal combustion emissions particularly from Indonesia. Consequently, using Pb isotopic fingerprints and elemental ratios, we find that the primary sources of atmospheric Pb are vehicular & ship emissions, heavy oil combustion, transboundary coal combustion emissions, waste incineration and recirculation of historic leaded gasoline.