Flexible, transparent and mechanically robust surface enhanced Raman scattering (SERS)-active substrates is currently the most attractive research focus in the field of Raman detection, and also a powerful analysis and identification technique in the biological research. Herein, we introduced a low-cost and large-scale method to fabricate flexible and transparent AgNPs/WPU plasmonic metafilm with monolayer-island phase nanostructures based on silver nanoparticles (AgNPs) and waterborne polyurethane emulsion (WPU) film. The obtained AgNPs/WPU plasmonic metafilm demonstrated excellent SERS sensitivity, signal uniformity and reproducibility, and the SERS substrates could still maintain excellent stability even after being bent or stretched over 100 cycles. The detection concentration was as low as 10 -9 M with 4-Mercaptobenzoic acid (4-MBA) as probe molecule, and the enhancement factor was high to 2.2×10 7 . More importantly, the flexibility and adhesivity of AgNPs/WPU plasmonic metafilm could be directly conformal coverage on the apple surface for in situ detection of thiram residue, and the detection limit was as low as 9.0165 ng cm −2 . This versatile AgNPs/WPU plasmonic metalfilm would be a promising SERS substrate for the detection of pesticide residue in chemical and biological applications.

Considering the inherent hydrophilic and porous nature of paper, the rapid absorption and diffusion of aqueous analyte solutions on paper-based SERS substrates may severely affect the Raman detection sensitivity and accuracy in the detection of target molecules. In this work, a series of hydrophobic CFP@PDA@AuNPs stripes were obtained through in situ synthesizing of gold nanoparticles (AuNPs) on a polydopamine (PDA)-decorated cellulose filter paper (CFP) and functionalized with perfluorodecanethiol (PFDT). When the SERS performance of the substrates was examined using 4-ATP, the hydrophobic CFP@PDA@AuNPs substrate showed superior sensitivity, reproducibility and stability due to the hydrophobic enrichment effect, with the detection limit decreasing to 10−9 M and the enhancement factor as high as 2.55 × 107. More importantly, it was feasible to apply the hydrophobic paper substrate as an excellent SERS sensor to detect methylene blue (MB) residues in lake water in a highly sensitive manner. The lowest detectable limit of MB was 100 nM, and it showed a low relatively standard deviation (RSD) value of 5.28%. Hydrophobic CFP@PDA@AuNPs stripes may serve as excellent sensors for target molecule detection and have tremendous potential in food security, and environmental and chemical detection.

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