Polycyclic aromatic hydrocarbons (PAHs) are a type of typical environmental pollutant with carcinogenic effects and high ecological risk. With the development of industry, surface water acts as a primary sink for PAHs. Owing to their low solubility, a significant amount of PAHs are adsorbed onto suspended particulate matter in surface water, which presents a serious risk to human health and the ecological environment. To protect human health and aquatic organisms, a systematic assessment of the trends in PAHs exposure risk is essential. Based on long-term monitoring data from 2002 to 2016, this study systematically evaluated the spatiotemporal distribution and source apportionment of PAHs adsorbed on suspended particulate matter in surface water. The results of the Mann-Kendall test indicated that pollution levels of PAHs decreased from 2012 to 2016. The maximum average content was 6239 μg·kg-1, and the minimum was 2760 μg·kg-1. Benzo(b)fluoranthene, benzo(k)fluoranthene, chrysene, and benzo(a)anthracene showed significant declines from 2002-2016 (P<0.05). Levels of benzo(a)pyrene, dibenzo(a,h)anthracene, and indeno(1,2,3-cd)pyrene were steady. Wavelet analysis showed that the pollution level of PAHs had significant periodic oscillations for surface water. Midstream and downstream Σ16PAHs showed significant declines from 2002-2016 (P<0.05), whereas upstream Σ16PAHs were steady. ANOVA analysis showed that the spatial difference was significant and occurred in the following order:midstream (6168 μg·kg-1)>upstream (5407 μg·kg-1)>downstream (3412 μg·kg-1). Diagnostic ratio analysis and the positive matrix factorization model suggested that the major sources of PAHs were traffic sources, coal burning sources, and biomass combustion sources, which accounted for 40.9%, 33.7%, and 25.4%, respectively. The contribution of traffic sources decreased by 25.9%. The contributions of coal burning sources and biomass combustion sources increased by 4.8% and 21.1% from 2002-2009 to 2010-2016, respectively. These results provide scientific reference for risk analysis and the control of PAHs pollution in surface water.
Keywords: polycyclic aromatic hydrocarbons(PAHs); source apportionment; temporal and spatial variation characteristics; uncertainty analysis; wavelet analysis.