Mechanically Robust Poly(ionic liquid) Block Copolymers as Self-Assembling Gating Materials for Single-Walled Carbon-Nanotube-Based Thin-Film Transistors AITranslate

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DOI：https://doi.org/10.1021/acsapm.2c02223

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The proliferation of high-performance thin-film electronics depends on the development of highly conductive solid-state polymeric materials. We report on the synthesis and properties investigation of well-defined cationic and anionic poly(ionic liquid) AB–C type block copolymers, where the AB block was formed by random copolymerization of highly conductive anionic or cationic monomers with poly(ethylene glycol) methyl ether methacrylate, while the C block was obtained by post-polymerization of 2-phenylethyl methacrylate. The resulting ionic block copolymers were found to self-assemble into a lamellar morphology, exhibiting high ionic conductivity (up to 3.6 × 10–6 S cm–1 at 25 °C) and sufficient electrochemical stability (up to 3.4 V vs Ag+/Ag at 25 °C) as well as enhanced viscoelastic (mechanical) performance (storage modulus up to 3.8 × 105 Pa). The polymers were then tested as separators in two all-solid-state electrochemical devices: parallel plate metal–insulator–metal (MIM) capacitors and thin-film transistors (TFTs). The laboratory-scale truly solid-state MIM capacitors showed the start of electrical double-layer (EDL) formation at ∼103 Hz and high areal capacitance (up to 17.2 μF cm–2). For solid-state TFTs, low hysteresis was observed at 10 Hz due to the completion of EDL formation and the devices were found to have low threshold voltages of −0.3 and 1.1 V for p-type and n-type operations, respectively.