Shift from legacy to emerging per- and polyfluoroalkyl substances for watershed management along the coast of China

Per- and polyfluoroalkyl substances and their short-chain alternatives have attracted world-wide attention due to their widespread presence and persistence in the environment. However, the sources, environmental fate, and driving forces of PFAS in coastal ecosystems remain poorly understood. In this study, the spatial distribution, source apportionment, and driving mechanisms of PFAS were investigated through a comprehensive analysis of water samples collected along the China's coastline. The concentrations of Sigma(25)PFAS in water samples followed a general pattern, with higher levels observed in northern coastal zones of China than the south, ranging from 0.72 to 1872.21 ng L-1. PFOA and PFBA were dominant. Emerging short-chain PFAS, such as PFBS, PFBA, F-53B and GenX, were frequently detected, with detection rates of 97%, 99%, 95% and 77%, respectively. This indicated a shift in coastal PFAS contamination from legacy compounds to emerging short-chain alternatives. Source apportionment using the Positive Matrix Factorization model identified key contributors to PFAS pollution, including textile production, volatile precursors, precious metal industries, aqueous film-forming foam, metal-plating, electrochemical fluorination, and fluoropolymer manufacturing. Additionally, PFAS concentrations were significantly positively correlated with cultivated land, urban area, and wastewater discharge, while negatively correlated with annual precipitation and woodland coverage (p < 0.05). Socio-economic development was identified as a major driver of PFAS emissions, while the hydrological factors and vegetation coverage can significantly enhance watershed resilience against PFAS pollution.