A low interfacial contact resistance is a challenge in polymer nanocomposites based on conductive nanomaterials for high-performance wearable electrode applications. Herein, a polydimethylsiloxane (PDMS)-based flexible nanocomposite incorporating high-conductivity 1D single-walled carbon nanotubes (SWCNTs) and 2D reduced graphene oxide (r-GO) was developed for high-performance electrocardiogram (ECG) wearable electrodes. A PDMS-SWCNT (P-SW; type I) nanocomposite containing only SWCNTs (2 wt%), exhibited rough and non-uniform surface morphology owing to the strong bundling effect of as-grown SWCNTs and randomly entangled aggregate structures and because of inefficient vacuum degassing (i.e., R P-SW = 1871 Ω). In contrast, owing to the hybrid structure of the SWCNTs (1 wt%) and r-GO (1 wt%), the PDMS-SWCNTs/r-GO (P-SW/r-GO; type II) nanocomposite exhibited uniform surface characteristics and low contact resistance (i.e., R P-SW/r-GO = 63 Ω) through the formation of hybrid and long conducting pathways. The optimized nanocomposite (P-SW/r-GO/f; type III) possessed a fabric-assisted structure that enabled tunable and efficient vacuum degassing and curing conditions. Additionally, a long and wide conducting pathway was formed through more uniform and dense interconnected structures, and the contact resistance was drastically reduced (i.e., R P-SW/r-GO/f = 15 Ω). The performance of the electrodes fabricated using the optimized nanocomposites was the same or higher than that of commercial Ag/AgCl gel electrodes during real-time measurement for ECG Bluetooth monitoring. The developed high-performance hybrid conducting polymer electrodes are expected to contribute significantly to the expansion of the application scope of wearable electronic devices and wireless personal health monitoring systems.
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