The electroanalytical wave against forever chemicals: molecularly imprinted electrochemical sensors for PFAS...

Per- and polyfluoroalkyl substances (PFAS) present a uniquely a formidable analytical challenge: ultra-trace regulatory limits, structural diversity spanning thousands of compounds, global environmental distribution, and established toxicological and regulatory concern. The persistence of these compounds, rooted in the strength of the carbon-fluorine bond, has driven drinking water thresholds into the low parts-per-trillion (ppt) range, transforming the scale and speed at which environmental measurement must operate. Liquid chromatography-tandem mass spectrometry delivers the required sensitivity and selectivity, but its laboratory-bound infrastructure cannot meet the geographic and temporal density that contemporary contamination management demands. Molecularly imprinted polymer (MIP)-based electrochemical sensors have emerged as a promising complementary strategy, pairing synthetic molecular recognition with the compact instrumentation and quantitative signal output of electrochemical transduction. even the most complete arrays, however, address only the targeted fraction of the PFAS burden that bulk organofluorine measurements reveal. This review critically examines the chemical diversity of PFAS, surveys established and emerging analytical platforms alongside their principal limitations, and evaluates the design principles governing MIP-based electrochemical sensors, including recent advances in sub-ppt detection validated in spiked river-water matrices, mediator-free detection using ambient dissolved oxygen, quantitative interferent modeling, and multiplexed instrumentation. Remaining challenges of matrix robustness, regeneration, breadth of PFAS coverage, standardized performance validation, and autonomous deployment are discussed within a tiered monitoring framework in which electrochemical sensors complement rather than replace established laboratory methods.