Organic electrochemical transistors (OECTs) are
signal transducers offering high amplification, which makes them particularly
advantageous for detecting weak biological signals. While OECTs typically
operate with aqueous electrolytes, those employing solid-like gels as the
dielectric layer can be excellent candidates for constructing wearable
electrophysiology probes. Despite their potential, the impact of the gel
electrolyte type and composition on the operation of the OECT and the
associated device design considerations for optimal performance with a chosen
electrolyte have remained ambiguous. In this work, we investigate the influence
of three types of gel electrolytes─hydrogels, eutectogels, and iongels, each
with varying compositions on the performance of OECTs. Our findings highlight
the superiority of the eutectogel electrolyte, which comprises poly(glycerol
1,3-diglycerolate diacrylate) as the polymer matrix and choline chloride in
combination with 1,3-propanediol deep eutectic solvent as the ionic component.
This eutectogel electrolyte outperforms hydrogel and iongel counterparts of
equivalent dimensions, yielding the most favorable transient and steady-state
performance for both p-type depletion and p-type/n-type enhancement mode
transistors gated with silver/silver chloride (Ag/AgCl). Furthermore, the
eutectogel-integrated enhancement mode OECTs exhibit exceptional operational
stability, reflected in the absence of signal-to-noise ratio (SNR) variation in
the simulated electrocardiogram (ECG) recordings conducted continuously over a
period of 5 h, as well as daily measurements spanning 30 days. Eutectogel-based
OECTs also exhibit higher ECG signal amplitudes and SNR than their
counterparts, utilizing the commercially available hydrogel, which is the most
common electrolyte for cutaneous electrodes. These findings underscore the
potential of eutectogels as a semisolid electrolyte for OECTs, particularly in
applications demanding robust and prolonged physiological signal monitoring.