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An auto-deformable supercapacitor which is composed of PPy(DBS) film (PPy doped with dodecyl benzene sulfonate anions, DBS−), reduced graphene oxide (rGO) film and Polyvinyl alcohol (PVA) gel electrolyte is fabricated. Benefiting from the synergy of flexible film electrodes and gel electrolyte, the volumetric effect of PPy(DBS) film produced by capacitance reaction is collected continually. The accumulated volumetric effect enables the as-designed supercapacitor to deform autonomously during the cyclic energy storage processes and generates more electrochemical active sites in PPy(DBS) film, which provides higher energy storage capacity for the supercapacitor. • Volumetric effect of PPy is collected and accumulated by synergy of flexible electrode and solid-state electrolyte. • The cumulative volumetric effect is applied to auto-deformable supercapacitor. • There is a quantitative relationship between the deformation degree and the capacitance. Polypyrrole (PPy) is one of the most extensively studied conducting polymers and it has promising application prospects in supercapacitors. However, PPy-based supercapacitors generally suffer from poor cycling stability due to the volumetric effect induced by ion doping/de-doping during the redox reactions. Therefore, the volumetric effect has usually been considered deleterious for supercapacitor applications. Herein, we demonstrate that the volumetric effect of PPy can be collected by synergy of flexible electrodes and solid-sate electrolytes. Furthermore, the accumulative volumetric effect is utilized in auto-deformable supercapacitors for the first time. The as-designed supercapacitor consists of flexible electrodes (PPy film, reduced graphene oxide (rGO) film) and a polyvinyl alcohol (PVA) gel electrolyte. When the redox reaction starts, the volumetric change of the PPy film induced by Na+ ion insertion is captured by the PVA gel electrolyte, resulting in mechanical deformation of the supercapacitor. As the accumulative volumetric effect drives greater deformation of the device, more electrochemically active sites are generated in the PPy film, leading to a higher energy storage capacity of the supercapacitor. Specifically, a certain correlation exists between the deformation degree and the energy storage capacity. As the deformation degree approaches 100% from 0%, the discharge capacity increases to 359 mF/cm3 from 101 mF/cm3. This auto-deformation characteristic endows the supercapacitor with subjective initiative, which establishes an important foundation for a smart energy storage device. [ABSTRACT FROM AUTHOR]

Self-standing film with desirable properties is a promising candidate for flexible electronic applications. Conducting polymers (CP) have intrinsic film forming and pseudocapacitive characteristics. However, pure CP films are rarely applied in energy storage devices due to their disordered molecular structure which would result in insufficient utilization of the supported active materials and apparent volumetric effect. The specific lamellar structure of 2D nanosheets is an ideal platform for CP growing into self-standing film with desirable structure. Herein, a facile interface engineering strategy is proposed for in-situ integrating 2D MoS 2 nanosheets into 3D polypyrrole (PPy) framework, in which dodecylbenzene sulfonate (DBS−) anions intercalate into MoS 2 nanosheets and guide PPy to grow into ordered molecular structure. The resultant self-standing films with PPy chains in a high degree of ordering can deliver a high area capacitance of 1200 mF/cm2 and a high volumetric capacitance of 325 F/cm3, which are significantly superior to pure PPy films and show a great potential for high performance flexible supercapacitor application. Image 1 [ABSTRACT FROM AUTHOR]