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

Daniil R Nosov; Bahar Ronnasi; Elena I Lozinskaya; Denis O Ponkratov; Laura Puchot; Patrick Grysan; Daniel F Schmidt; Benoît H Lessard; Alexander S Shaplov

doi:10.1021/acsapm.2c02223

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

ACS Appl Polym Mater. 2023 Mar 30;5(4):2639-2653. doi: 10.1021/acsapm.2c02223. eCollection 2023 Apr 14.

Authors

Affiliations

¹ Luxembourg Institute of Science and Technology (LIST), 5 Avenue des Hauts-Fourneaux, L-4362 Esch-sur-Alzette, Luxembourg.
² Department of Physics and Materials Science, University of Luxembourg, 2 Avenue de l'Université, L-4365 Esch-sur-Alzette, Luxembourg.
³ Department of Chemical & Biological Engineering, University of Ottawa, 161 Louis Pasteur, Ottawa, Ontario K1N 6N5, Canada.
⁴ A.N. Nesmeyanov Institute of Organoelement Compounds Russian Academy of Sciences (INEOS RAS), Vavilov str. 28, bld. 1, 119334 Moscow, Russia.
⁵ School of Electrical Engineering and Computer Science, University of Ottawa, 800 King Edward Avenue, Ottawa, Ontario K1N 6N5, Canada.

Abstract

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.