Size distributions of source-specific risks of atmospheric heavy metals: An advanced method to quantify source contributions to size-segregated respiratory exposure

Highlights: • Heavy metals in size-segregated particulate matter were measured in an industrial megacity. • A model was developed to quantify source-specific risk of size-segregated particulate matter. • Industrial emission is a key contributor of risks, and its size distribution was bimodal. • Coal combustion contributed higher risks in small PM and during autumn and winter. • Resuspended dust contributed higher risks in coarse PM and during spring and summer. Heavy metals in size-segregated particulate matter (PM) were investigated in a Chinese megacity, and an advanced model was developed to quantify source-specific risks focusing on size-segregated respiratory exposure. Incremental lifetime cancer risk (ILCR) and non-cancer risk (hazard quotient: HQ) based on deposition concentrations of heavy metals displayed a peak at 4.7–5.8 µm. The percentage contributions to cancer risk were as follows: industrial emission (IE, 34%) > secondary and transport (ST, 29%) > resuspended dust (RD, 21%) > coal combustion (CC, 11%) > traffic emission (TE, 4%) during spring and summer (SS), and CC (31%) > ST (26%) > IE (21%) > RD (11%) ≈ TE (11%) during autumn and winter (AW). RD (41% of HQ during SS, 28% during AW) and IE (45% of HQ during SS, 35% during AW) dominated non-cancer risk. ILCR and HQ of CC were high at sizes 1.1–2.1 µm and 0.43–0.65 µm; those of RD were high at sizes > 3.3 µm; and those of IE were bimodal at fine (2.1 µm) sizes, respectively. Cancer risk was more susceptible to small particles than non-cancer risk, partly because higher ILCR was from CC, but higher HQ was attributed by RD.