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Hollow Microneedle-based Sensor for Multiplexed Transdermal Electrochemical Sensing
Published on: June 1, 2012
Laser-written high-entropy metal-oxy patch for non-enzymatic lactate-pH sweat sensing
Liang Fan1, Jianru Wang1, Yuxiang Xin1
1School of Chemistry and Chemical Engineering, Hubei Key Laboratory of Bioinorganic Chemistry and Materia Medica, Hubei Engineering Research Center for Biomaterials and Medical Protective Materials, Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education Huazhong University of Science and Technology (HUST), Wuhan, 430074, PR China; Guangdong HUST (Huazhong University of Science and Technology) Industrial Technology Research Institute, Dongguan, 523808, PR China.
None:
Wearable sweat analytics demands sensing interfaces that remain catalytically active in biofluids yet are manufacturable in flexible formats. Here we report a one-step CO2-laser writing strategy that converts chitosan-multimetal precursor on polyimide into a porous N-doped graphene (NG) network uniformly anchored with high-entropy multimetal (oxy)nanoparticles (HEMO). The laser process yields a high-entropy (oxy)surface where metallic ensemble sites coexist with oxygenated motifs (M-O/M-OH), generating mixed-valence catalytic centers electronically coupled to the conductive graphene. Leveraging this architecture, the flexible electrode enables lactate-pH co-sensing under neutral conditions. Non-enzymatic lactate detection proceeds via adsorption-assisted electrocatalytic oxidation on multimetal ensemble sites, where the mixed-valence (oxy)surface accelerates interfacial charge transfer and turnover, delivering a linear range of 0.05-20 mM with a detection limit of 8.83 μM. Concurrently, potentiometric pH sensing arises from reversible proton-coupled conversion between -OH and -O-∗ on oxygenated surface groups, producing a linear open-circuit potential (OCP)-pH relationship. Finally, integrating the laser-written electrodes into a skin-conformal patch with microfluidics and wireless electronics enables real-time exercise monitoring, tracking sweat lactate dynamics with pH shifts and agreeing well with standard reference assays. Collectively, this work establishes a scalable, laser-enabled route to high-entropy metal-oxy electrocatalytic interfaces for pH-assisted lactate quantification and multiplexed wearable sweat sensing.
