A molecularly imprinted electrochemical microneedle sensor for multiplexed metabolites detection in human sweat

This article demonstrates an array of inexpensive molecularly imprinted microneedle platforms for the multiplexed electrochemical detection of pH, epinephrine, dopamine, and lactate biomarkers in human sweat. The multiplexed sensors were fabricated via layer-by-layer (LbL) assembly on a polydimethylsiloxane (PDMS) microneedle platform coated with a conductive PDMS/carbon nanotube (CNT)/cellulose nanocrystal (CNC) composite (PDMS/CNT/CNC@PDMS). The pH sensor was comprised of a pH-responsive polyaniline (PANI)/CNT/CNC/silver nanoparticle (AgNP) composite layer. The epinephrine, dopamine, and lactate sensors consisted of an additional epinephrine, dopamine, or lactate-imprinted PANI-co-3-aminophenylboronic acid (PBA)/gold nanoparticle (AuNP) layer atop the PANI/CNT/CNC/AgNP composite layer. Each sensor rapidly (∼2 min) and selectively responded to their target analytes, with excellent precision between scans. The limits of detection (LOD) for the epinephrine, dopamine, and lactate sensors were 0.0007 ± 0.0002 μM, 2.11 ± 0.05 nM, and 0.07 ± 0.07 mM, respectively. The pH sensor accurately responded to a pH range of 4.25-10. The applicability of the sensor platforms were successfully verified through quantification of pH, epinephrine, dopamine, and lactate in a human sweat sample, showing promise for use as a wearable, point of need (PON) sensor for sweat analytics.