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Summary: As one kind of conducting polymer composite, poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) has been widely used as an electrode for energy storage and conversion devices because of its optical transmittance, flexibility, and high electrical conductivity etc. Here, we prepared binding‐free PEDOT:PSS fibers (PFs) electrodes with high capacitive performance for supercapacitors via a facile method followed by various solvent treatments. Dimethyl sulfoxide (DMSO)‐treated electrodes displayed a better specific capacitance (Cs) of 202 F/g at 0.5 A/g with higher elongation at break, flexibility, and conductivity of 140.7 S/cm, compared to those of pristine PEDOT:PSS materials. More importantly, the DMSO‐treated fibers possessed improved stability, which retained 105% of the initial Cs after 22 000 long cycles at 10 A/g. It is believed that the fabricated PFs will be promising organic electrodes for portable supercapacitors and other flexible electronic devices in the near future. [ABSTRACT FROM AUTHOR]

Adjusting the assembly of EDOT monomers through different oxidants can improve the structure and electrochemical performance of PEDOT. [Display omitted] • Explored different initiators to induce monomer assembly. • High oxidation degree and long conjugated chain of PEDOT achieved by Fe(Tos) 3. • PEDOT/P(Fe(Tos) 3)-6 displayed high areal capacitance of 419 mF cm-2 at 1 mA cm-2. The development of poly(3,4-ethylenedioxythiophene) (PEDOT) with high specific capacitance is the key to pursuing high-performance supercapacitors, and the electrochemical properties of PEDOT are closely related to the oxidation degree and conjugated chain length of its molecular chain. In this work, the influences of various oxidants (FeCl 3 , Fe(Tos) 3 and MoCl 5) on the molecular chain structure and capacitive properties of PEDOT via vapor phase polymerization were systematically investigated. Fe(Tos) 3 can significantly improve the degree of oxidation and the length of the conjugated chain of PEDOT compared to FeCl 3 and MoCl 5 , enhancing the conductivity and providing more active sites for Faraday reaction. Therefore, the PEDOT/P(Fe(Tos) 3) electrode displays a considerable conductivity of 73 S cm-1, high areal capacitance (419 mF cm-2) and excellent electrochemical stability under the different bent state. Moreover, the conjugated structure strengthens the interaction between PEDOT chains, achieving good cycle stability. Therefore, Fe(Tos) 3 is an ideal oxidant for obtaining high-performance PEDOT electrode materials. [ABSTRACT FROM AUTHOR]

Flexible PEDOT/paper with high electrochemical performance and excellent stability was successfully fabricated for supercapacitor. • The PEDOT/paper was prepared via vapor phase polymerization. • PEDOT/paper showed excellent flexibility and stability. • PEDOT/paper displayed high areal capacitance of 639 m F cm−2 at 1 mA cm-2. • PEDOT/paper displayed high specific capacitance of 118 F g−1 at 1 mA cm-2. Currently, electrodes with favorable flexibility, high capacitance and conductivity is vital to the development of supercapacitors. However, it is still a great challenge to manufacture these materials simply and inexpensively. Herein, vapor phase polymerization (VPP) is applied in this work to deposit poly(3,4-ethylenedioxythiophene) (PEDOT) on the flexible paper, which can prepare electrode on a large scale. The fabricated PEDOT/paper possesses porous structure, which can facilitate sufficient contact between electrolyte and electrode material, and benefit for ions diffusion. The effect of different amount of PEDOT on the electrochemical properties of the PEDOT/paper is investigated. As expected, the prepared electrode exhibits high areal capacitance of 639 m F cm−2 and good conductivity of 78 S cm-1, remarkable stability under different bending angle conditions, which can be directly used as electrode for flexible and light-weight energy storage devices. It is believed that the method is useful to improve both electrical conductivity and capacitance of the PEDOT/paper, and further to optimize the electrochemical performance of the prepared material. [ABSTRACT FROM AUTHOR]