Compound-specific radiocarbon analysis of polycyclic aromatic hydrocarbons (PAHs) in sediments from an urban reservoir

A quantitative apportionment of polycyclic aromatic hydrocarbons (PAHs) derived from fossil fuel combustion (C-14-free) and biomass burning (contemporary C-14) was carried out using a recently developed compound-specific radiocarbon analysis (CSRA) method for a sediment core from an urban reservoir located in the central Tokyo metropolitan area, Japan. The C-14 abundance of PAHs in the sediments was measured by accelerator mass spectrometry (AMS) after extraction and purification by three types of column chromatography, by high performance liquid chromatography (HPLC), and, subsequently, by a preparative capillary gas chromatography (PCGC) system. This method yielded a sufficient quantity of pure compounds and allowed a high degree of confidence in the determination of C-14. The fraction modern values (f(M)) of individual PAHs (phenanthrene, alkylphenanthrenes, fluoranthene, pyrene and benz[a]anthracene) in the sediments ranged from 0.06 to 0.21. These results suggest that sedimentary PAHs (those compounds mentioned above) were derived mostly from fossil fuel combustion. Three sectioned-downcore profiles (similar to40 cm) of the C-14 abundance in phenanthrene and alkylphenanthrenes showed a decreasing trend with depth, that was anti-correlated with the trend of SigmaPAHs concentration. The f(M) values of phenanthrene were also larger than those of alkylphenanthrenes in each section of the core. This result indicates that phenanthrene received a greater contribution from biomass burning than alkylphenanthrenes throughout the core. This finding highlights the method used here as an useful approach to elucidate the source and origin of PAHs in the environment. (C) 2004 Elsevier B.V. All rights reserved.