| In recent years,with the vigorous development of science and technology,the continuous upgrading of electronic equipment has led to the rapid rise of personalized flexible electronic equipment,which has further promoted the rapid development of flexible energy storage devices.Then,compared with traditional flexible energy storage devices,all-in-one energy storage devices have good electrochemical performance and strong anti-deformation ability,and broader application prospects in the field of flexible electronics.However,the reported all-in-one energy storage devices have some disadvantages,such as low utilization rate of active materials,poor cycle performance,unstable structure,and so on.Therefore,this thesis optimizes the electrochemical stability of the polyaniline active material,the ionic-electron conductivity of the polyaniline membrane electrode,and the assembly process of polyaniline based all-in-one energy storage devices.Thus,polyaniline based active materials,flexible membrane electrode,and flexible all-in-one energy storage device with excellent performance are prepared.The specific research content includes:(i)In order to obtain polyaniline based active materials with good electrochemical stability,polyaniline based conductive polymers are modified by monomer copolymerization.Change the monomer ratio to obtain different conductive polymers through the analysis of the structure,band gap width of the samples,and simulating the electronic cloud deployment(HOMO-LUMO)with density functional theory(DFT).Then the electrochemical performance is tested.And carbonizing the conductive polymer to obtain the carbon materials,which also has excellent electric double layer capacitance.Then,they are assembled into asymmetric supercapacitors,and after 5000 cycles,the specific capacity can still maintain 80.4%of the initial specific capacity.Subsequently,Zn2+battery assembled with conductive polymer also has good electrochemical performance.(ii)In order to obtain polyaniline based membrane electrode materials with high utilization rate of active substances,the monomers and good electronic conductors are in-situ introduced into the gel phase,and the conductive polymer substrate membrane electrode materials are obtained by in-situ polymerization to enhance the ion electron transport rate of polyaniline and obtain conductive polymer base membrane electrode materials with high conductivity and specific capacitance.In this experiment,the active materials(PANI/PPY)and good electron conductors(Au NP/Ag NP)are in-situ introduced into the electrolyte membrane to construct the ionic-electronic conductivity networks to increase the active sites of the active materials.And by designing four different membrane electrodes and electrolytes to verify the existence of the dual-conductivity networks.Subsequently,the polymerization time of active material and the amount of good electron conductor are optimized,and the conductivity of membrane electrode is tested.Finally,the membrane electrode with dual conductivity network is introduced into the supercapacitor,and the effect on the electrochemical performance is studied.(iii)In the above chapters,the active materials and membrane electrodes are optimized.However,when assembling energy storage devices,water system and pressed structure are used,which greatly limits the wearability and portability of energy storage devices.Therefore,in order to obtain the portability and high mechanical properties of polyaniline based flexible all-in-one energy storage devices,the interfacially cross-linking strategy with the substrate and interface is used to improve the stability of the electrode-electrolyte interface to obtain portable energy storage with high mechanical properties and high electrochemical properties.In this experiment,the gel electrolyte is used as the substrate of the membrane electrode,and as the cross-linking agent between the membrane electrodes.Under the chelating action of metal ions,the“electrode-electrolyte-electrode”is cross-linked into a whole.Under this strategy,the energy storage device has smaller intrinsic impedance(Rs=1.82Ω)and mechanical stability;more importantly,it enables the supercapacitor to be used as a common module to achieve arbitrary,designable and multi-dimensional integration to adapt to the complex power supply system.This strategy has also been successfully applied to other energy storage devices(PVA based supercapacitor,Zn-MnO2 battery). |