National inventory of perfluoroalkyl substances in archived U.S. biosolids from the 2001 EPA National Sewage Sludge Survey

•First study to report nationwide occurrence and concentrations of perfluoroalkyl substances (PFAS) in U.S. biosolids.•Ten out of thirteen PFAS analyzed were consistently detected in all biosolids samples.•PFOS was the most abundant PFAS in biosolids, followed by PFOA.•Mean load of ∑PFASs in U.S. biosolids was estimated at 2749–3450kg/year.•PFASs in biosolids show no significant difference between pre- and post-phase out period. Using liquid chromatography tandem mass spectrometry, we determined the first nationwide inventories of 13 perfluoroalkyl substances (PFASs) in U.S. biosolids via analysis of samples collected by the U.S. Environmental Protection Agency in the 2001 National Sewage Sludge Survey. Perfluorooctane sulfonate [PFOS; 403±127ng/g dry weight (dw)] was the most abundant PFAS detected in biosolids composites representing 32 U.S. states and the District of Columbia, followed by perfluorooctanoate [PFOA; 34±22ng/gdw] and perfluorodecanoate [PFDA; 26±20ng/gdw]. Mean concentrations in U.S. biosolids of the remaining ten PFASs ranged between 2 and 21ng/gdw. Interestingly, concentrations of PFOS determined here in biosolids collected prior to the phase-out period (2002) were similar to levels reported in the literature for recent years. The mean load of ∑PFASs in U.S. biosolids was estimated at 2749–3450kg/year, of which about 1375–2070kg is applied on agricultural land and 467–587kg goes to landfills as an alternative disposal route. This study informs the risk assessment of PFASs by furnishing national inventories of PFASs occurrence and environmental release via biosolids application on land.