For foldable electronic devices of the future, most components should have very good flexibility and reliability to maintain electrical properties even under repeated deformation. In this study, two types of inks for conducting polymer and graphene were simultaneously printed on flexible plastic substrates via the newly developed consecutive ink writing (CIW) process for the formation of composite electrodes of foldable electronic devices. To consecutively print conducting polymer ink and graphene ink, a conventional three-dimensional (3D) printer was modified by installing two needles in the printer head, and the two inks were printed through the nozzle in the same route with a time interval. By adjusting several printing conditions (ink concentration, printing parameters, printing time intervals between the two inks, etc.), various structures of composite electrodes, such as layered or fused 2D or 3D structures were developed on the glass substrate. Furthermore, by changing the printing order of the two inks and 3D printer bed temperature, the composite electrodes with a higher printing resolution were successfully printed on the flexible polyimide substrate. The printed composite electrodes via CIW process exhibit the lowest surface electrical resistance of 0.9 kΩ and high flexibility, and stable resistance values were maintained after 1000 cycles of the folding test. Consequently, the CIW process developed in this study applies to the production of the electrical parts and components for various flexible devices, such as foldable and wearable electronics.
Keywords: 3D printing; composite; conducting polymer; electrode; graphene.