Zinc-ion hybrid supercapacitors(ZHSs)are promising energy storage systems integrating high energy density and high-power density,whereas they are plagued by the poor electrochemical stability and inferior kinetics of ...Zinc-ion hybrid supercapacitors(ZHSs)are promising energy storage systems integrating high energy density and high-power density,whereas they are plagued by the poor electrochemical stability and inferior kinetics of zinc anodes.Herein,we report an electrolyte additive-assembled interconnecting molecules-zinc anode interface,realizing highly stable and fast-kinetics zinc anodes for ZHSs.The sulfobutyl groups-graftedβ-cyclodextrin(SC)supramolecules as a trace additive in ZnSO_(4)electrolytes not only adsorb on zinc anodes but also self-assemble into an interconnecting molecule interface benefiting from the mutual attraction between the electron-rich sulfobutyl group and the electron-poor cavity of the adjacent SC supramolecule.The interconnecting molecules-zinc anode interface provides abundant anion-trapping cavities and zincophilic groups to enhance Zn^(2+)transference number and homogenize Zn^(2+)deposition sites,and meanwhile,it accelerates the desolvation of hydrated Zn^(2+)to improve zinc deposition kinetics and inhibit active water molecules from inducing parasitic reactions at the zinc deposition interface,making zinc anodes present superior reversibility with 99.7%Coulombic efficiency,~30 times increase in operation lifetime and an outstanding cumulative capacity at large current densities.ZHSs with 20,000-cycle life and optimized rate capability are thereby achieved.This work provides an inspiring strategy for designing zinc anode interfaces to promote the development of ZHSs.展开更多
基金the National Key R&D Program of China(2022YFB2404500)Guangdong Basic and Applied Basic Research Foundation(2023A1515110347+2 种基金2023A1515012087)Funding by Science and Technology Projects in Guangzhou(2024A04J3267)the Fundamental Research Funds for the Central Universities(21624411).
文摘Zinc-ion hybrid supercapacitors(ZHSs)are promising energy storage systems integrating high energy density and high-power density,whereas they are plagued by the poor electrochemical stability and inferior kinetics of zinc anodes.Herein,we report an electrolyte additive-assembled interconnecting molecules-zinc anode interface,realizing highly stable and fast-kinetics zinc anodes for ZHSs.The sulfobutyl groups-graftedβ-cyclodextrin(SC)supramolecules as a trace additive in ZnSO_(4)electrolytes not only adsorb on zinc anodes but also self-assemble into an interconnecting molecule interface benefiting from the mutual attraction between the electron-rich sulfobutyl group and the electron-poor cavity of the adjacent SC supramolecule.The interconnecting molecules-zinc anode interface provides abundant anion-trapping cavities and zincophilic groups to enhance Zn^(2+)transference number and homogenize Zn^(2+)deposition sites,and meanwhile,it accelerates the desolvation of hydrated Zn^(2+)to improve zinc deposition kinetics and inhibit active water molecules from inducing parasitic reactions at the zinc deposition interface,making zinc anodes present superior reversibility with 99.7%Coulombic efficiency,~30 times increase in operation lifetime and an outstanding cumulative capacity at large current densities.ZHSs with 20,000-cycle life and optimized rate capability are thereby achieved.This work provides an inspiring strategy for designing zinc anode interfaces to promote the development of ZHSs.