Rewritable paper has greatly promoted the sustainable development of society. However, the hydrophilicity/lipophilicity of the poly(3,4-ethylenedioxythiophene) (PEDOT) film limits its application as the rewritable paper. Herein, we constructed a repeatable writing/erasing pattern on a PEDOT film (rewritable PEDOT paper) by combining wettability control, water-induced dedoping, and an electrochemical redox reaction. The treatment with a medium-polarity/high-volatility solvent (MP/HVS) adjusted the wettability of the PEDOT film (water contact angle increased from 6.5° to 146.2°), contributing to the formation of a hydrophobic writable substrate. The treatment with a high-polarity solvent (HPS) induced the dedoping of anions in the PEDOT chain, resulting in the film's color changed from blue to purple and serving as a writing process. The intrinsic electrochemical redox (elimination of color change by doping/dedoping of lithium ions in the PEDOT chain) of the PEDOT film enabled the erasing process. This writing/erasing process can be repeated at least 10 times. The patterned PEDOT film maintained excellent stability to standing diverse solvents (low-polarity solvent (LPS) and MP/HVS), high temperatures (350 °C), and irradiation of different light wavelengths (wavelengths of 365, 380, 460, 520, and 645 nm). Additionally, the conductivity of the PEDOT film was quantitatively measured (impedance: LPS, increased 8.84%; MP/HVS, decreased 6.67%; and HPS, increased 27.97%) by fabricating a micropatterned PEDOT electrode. This work will provide a method for the fabrication of PEDOT-based optoelectronic functional materials.
Keywords: PEDOT film; doping/dedoping; rewritable paper; solvent-induced modulation; water-writing/electroerasing.