A perfluorinated sulfonic acid-based double-layered membrane-coated polymeric microneedle glucose sensor with wide linear range for long-term stable monitoring
Microneedle-based electrochemical patch sensors provide a minimally invasive and accurate approach for monitoring interstitial fluid (ISF) glucose levels. However, the existing patch-type sensors often suffer from limited detection range, poor stability, and temperature-dependent inaccuracies. In this study, we propose a polymeric microneedle-based glucose biosensor integrated with a temperature sensor that incorporates a double-layer fluorinated copolymer membrane coating using a combinatorial chemistry approach. The first membrane coating layer, composed of perfluorinated sulfonic acid (PSA)-modified cyclohexanol (ChA), preserves enzyme activity, whereas the second PSA layer serves as a diffusion-limiting barrier, both of which are applied using layer-by-layer dip-coating. The optimized glucose biosensor demonstrated excellent linearity in glucose response up to 35 mM, with a single linear fit and a high sensitivity of 18.46 μAmM-1cm-2. It exhibited an outstanding detection limit of 1.8 μM and maintained stable in-vitro performance for up to 28 days. In addition, a temperature-compensation algorithm was implemented to correct temperature-induced glucose reading variations. In-vivo validation of the biosensor in the rabbit model confirmed its reliability for stable ISF glucose monitoring. These results highlight the potential of the developed membrane-functionalized needle glucose biosensor as a robust platform for long-term, real-time, and wide-range ISF glucose tracking.
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