Rational design of viologen redox additives for high-performance supercapacitors with organic electrolytes

Introducing redox species into the electrolytes of traditional electric double layer capacitors(EDLCs)is an efficient strategy to enhance their energy density owing to Faradic reactions.However,few studies have elucidated the effect of the molecular structures of organic redox species on the performance of relative supercapacitors,which is important in the development of redox additives for super-capacitors.In this context,we synthesized several viologens and used them as new organic redox additives for super-capacitors with organic electrolytes.The detailed experimental analysis and theoretical calculation results show that the electrochemical performance of viologens relies heavily on their side chains and conjugated cores.Specifically,the side chains of the viologens affect their electronic structures and are consistent with behaviours between the molecules and the electrode pores due to the size effect,thus influencing their specific capacities.In addition,a larger conjugated aromatic core endows viologens with a smaller band gap and a higher degree of electron delocalization,resulting in better rate performance and cycling stability.Consequently,aπ-conjugated viologen derivative is selected as a favourable additive and enables an EDLC-type supercapacitor to exhibit a high energy density(34.0 W h kg^−1 at 856 W kg^−1)and good cycling performance.

Reversible faradaic reactions involving redox mediators and oxygen-containing groups on carbon fiber electrode for high-performance flexible fibrous supercapacitors

Flexible fibrous supercapacitors(FFS)are taking account of as the energy storage devices for wearable electronics owing to their high power density,high safety,long cycle life,and simple manufacturing process.Nevertheless,FFSs have the disadvantage of low specific capacitance that results from the electrochemical characteristics of the electrical double layer on the carbon fiber electrode.In this study,for the first time,an FFS comprising surface-activated carbon fibers as an electrode/current collector and a redox additive gel polymer electrolyte(FFS-SARE)was fabricated for use as a wearable energy storage device.The FFS-SARE showed outstanding electrochemical performance,namely,high specific capacitances of 891 and 399 mF cm^(-2) at current densities of 70.0 and 400 μA cm^(-2),respectively,and remarkable ultrafast cycling stability over 5000 cycles with 92%capacitance retention at a current density of 400.0 μA cm^(-2).Moreover,they exhibited mechanical flexibility and had high feasibility,and they showed good energy storage performance that renders them suitable for use in wearable electronic textiles.