Calculating sources of combustion-derived particulates using 1-nitropyrene and pyrene as markers

Airborne particulate matter (PM) contains numerous hazardous polycyclic aromatic hydrocarbons (PAHs) as well as their functionalized congeners. However, the lack of useful methods to identify the sources of PM has hindered the development of researches in atmospheric and public health fields. This report proposes a new method for estimating the source contribution of combustion-derived particulate (P_c) by using 1-nitropyrene (1-NP) and pyrene (Pyr) as markers. This is premised on the fact that the formation of nitrogen oxides in the flame gas and the subsequent nitration of PAHs are functions of combustion temperature and therefore the concentration ratios of NPAHs to PAHs are highly temperature dependent. This method divides combustion sources into two groups - high and low temperatures - which here are respectively represented by automobile engine and coal combustion in urban areas. Formulae are derived for combustion-derived particulate (P_c), whose fraction in the total particulate is y (0 < y < 1), and particulates from combustion sources with high temperatures (P_h), whose fraction in P_c is x (0 < x < 1), and low temperatures (P_l), whose fraction is (1 －x). When concentrations of 1-NP and Pyr in P_h and P_l are known, values x and y can be calculated from the formulae by determining atmospheric 1-NP and Pyr concentrations at monitoring sites. Then atmospheric concentrations of P_c, P_h and P_l can be calculated. The proposed method has been applied for total suspended particulate matter (TSP) samples collected in Kanazawa and Kitakyushu (Japan) and Beijing (China) having different types of atmospheric pollution to clarify the change of contributions of automobiles and coal combustion.