Pulse Sensors Based on Laser-Induced Graphene Transferred to Biocompatible Polyurethane Networks: Fabrication, Transfer Methods, Characterization, and Application

Flexible, wearable biomedical sensors based on laser-induced graphene (LIG) have garnered significant attention due to a straightforward fabrication process and exceptional electrical and mechanical properties. However, most relevant studies rely on commercial polyimide precursors, which suffer from inadequate biocompatibility and weak adhesion between the precursor material and the LIG layer. To address these challenges, we synthesized cross-linked polyurethanes (PUs) with good biocompatibility and used them as substrates for LIG-based wearable pulse sensors. During fabrication, we employed two methods of LIG transfer to achieve optimal transfer yield. We adjusted the thickness of PU films and tailored their mechanical and physicochemical properties by varying the soft segment content to achieve optimal sensor performance. Our findings demonstrate that the success of LIG transfer is strongly influenced by the structure and composition of the polymeric substrate. Tensile testing revealed that increasing the soft segment content in PU films significantly improved their tensile strength, elongation at break, and flexibility, with PU based on 50 wt.% soft segment content (PU-50) showing the best mechanical properties. LIG exhibited minimal sensitivity to humidity, while PU films maintained high transparency (>80% at 500 nm), and PU-50 was non-toxic, with less than 5% lactate dehydrogenase (LDH) release in endothelial cell cultures, confirming its biocompatibility. Adhesion tests demonstrated that LIG transferred onto PU-50 exhibited significantly stronger adhesion compared to other tested substrates, with only a 30% increase in electrical resistance after the Scotch tape test, ensuring stability for wearable sensors. The optimal substrate, a semicrystalline PU-50, yielded superior transfer efficiency. Among all tested sensors, the LIG/PU-50, featuring a 77 μm thick substrate with good mechanical properties and improved adhesion, exhibited the highest signal-to-noise ratio (SNR). This study showcases a skin-safe LIG/PU-based pulse sensor that has significant potential for applications as a wearable patch in medical and sports monitoring.