Two-layer Homolog Network Approach for PFAS Nontarget Screening and Retrospective Data Mining

The rapid increase of novel per- and polyfluoroalkyl substances (PFAS) raises concerns, while their identification remains challenging. Here, we develop a two-layer homolog network approach for PFAS nontarget screening using mass spectrometry. The first layer constructs networks between homologs, with evaluation showing that it filters 94% of false candidates. The second layer builds a network between classes to expedite the identification of PFAS. We detected 94 PFAS in twelve waterproof products and two related industrial sludges, including 36 novel PFAS not previously reported in any sample. A local dataset is constructed for retrospective analysis by re-analyzing our previous samples, revealing fifteen novel PFAS in samples collected in 2005. The retrieval of the public database MassIVE uncovers novel PFAS in samples from seven countries. Here, we reveal the historic and global presence of novel PFAS, providing guidance for the management and policy-making concerning persistent chemicals.