Abstract

In this work, we report large-area, semi-transparent, and flexible all-solid-state supercapacitors (ASSCs) fabricated using scalable D-bar coating, which is compatible with roll-to-roll printing processes. The poly (3,4-ethylenedioxythiophene):poly (styrene sulfonate) (PEDOT:PSS)-based transparent conducting electrodes (TCEs) show optical transparencies of T550nm > 85% and conductivities of ~3645 S cm−1. An ASSC device (~1 cm2) consists of D-bar coated TCEs and PVA/LiCl gel-electrolyte and exhibits a high areal capacitance per electrode (Ca) of 4.7 mF cm−2, which is about 35% higher than that of ASSC devices containing spin coated TCEs. A PEDOT:PSS ASSCs with the transparency of T550nm > 65% presents stable capacitance up to 10,000 charge/discharge cycles and 5000 bending cycles at a bending radius of 2 mm, demonstrating excellent electrochemical robustness and flexibility. Moreover, the large-area (~64 cm2) ASSC fabricated with D-bar coating exhibited a Ca of 2.9 mF cm−2, a maximum energy density of 18 µWh cm−2 and a power density of 1600 µW cm−2, which outperforms state-of-the-art transparent and flexible ASSCs. The agglomerated PEDOT:PSS nanofibrils and dipper pore size on D-bar coated TCEs, enables efficient ion adsorption/desorption and charge intercalation, which leads to the high performance of the flexible ASSC.

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