A stable dual-functional monomer imprinted polymer platform for electrochemical sensitive detection of PFAS

Electrochemical molecular imprinting technology (e-MIT) has gained significant attention for detecting emerging micropollutants like per- and polyfluoroalkyl substances (PFAS). However, designing efficient and reliable PFAS sensors based on e-MIT remains challenging. In this study, we explored a mechanism for synergistic adsorption recognition of dual-functional monomers (DM), based on which a molecularly imprinted electrochemical sensor with high sensitivity and stability was developed for PFOA detection. DFT simulations demonstrated that the synergistic interaction between DMs enhances both molecular adsorption capacity and structural stability. Response surface methodology was employed to optimize the MIP composition, revealing a strong correlation between the DM ratio and sensor performance. The optimized MIP-modified electrode exhibited a higher Langmuir adsorption coefficient (Kₐ = 8.92 × 10⁸ cm³ mol^-1) and improved stability (RSD < 2 %) compared to single-functional monomer electrodes. Additionally, Al/Co-MOFs/rGO complexes are coupled as the sensor basement. The sensor displayed a wide linear detection range (10 pM to 100 nM), low detection limit (5 pM), and excellent recoveries (94 %-107 %) in river samples, demonstrating its robustness and reliability in real-world applications. This study highlights the potential of DM-based electrochemical sensors for sensitive and reliable detection of emerging micropollutants in complex water environments, paving the way for future monitoring and environmental protection.