Zinc-iodine batteries have received significant attention due to their high theoretical capacity and environmental friendliness,but their performance is restricted by the growth of zinc dendrites,the hydrogen evolutio...Zinc-iodine batteries have received significant attention due to their high theoretical capacity and environmental friendliness,but their performance is restricted by the growth of zinc dendrites,the hydrogen evolution reaction,and the shuttling effect of polyiodide ions.In this study,an amidoximefunctionalized hydrogel electrolyte,created by amidoximated porous polymer of intrinsic microporosity(AO-PIM-1)and sodium alginate(Alg),is designed to address the aforementioned problems through synergistically optimizing the interfaces of the zinc anode and iodine cathode.The rigid microporous framework and amidoxime groups of AO-PIM-1 can repel polyiodides and inhibit their shuttle effect.Meanwhile,the polyanionic properties of Alg guide the uniform deposition of Zn^(2+)along the(002)crystal plane through the“egg-box”structure,thus suppressing the formation of dendrites.The AO-PIM-1/Alg electrolyte has a high ionic conductivity(18.6 mS cm^(-1)).The assembled symmetric battery can achieve highly reversible dendrite-free zinc plating/stripping(stably cycling for 2550 h at 1 mA cm^(-2)).The Zn-I_(2) full battery with the AO-PIM-1/Alg electrolyte has a long lifespan of 8700 cycles at 0.5 A g^(-1).The working mechanism of the electrolyte was elucidated through density functional theoretical calculations and molecular dynamics simulations.This study provides a new strategy for the hydrogel electrolyte of ZnI_(2) batteries.展开更多
Static rechargeable zinc-iodine(Zn-I_(2))batteries are superior in safety,costeffectiveness,and sustainability,giving them great potential for large-scale energy storage applications.However,the shuttle effect of poly...Static rechargeable zinc-iodine(Zn-I_(2))batteries are superior in safety,costeffectiveness,and sustainability,giving them great potential for large-scale energy storage applications.However,the shuttle effect of polyiodides on the cathode and the unstable anode/electrolyte interface hinder the development of Zn-I_(2)batteries.Herein,a self-segregated biphasic electrolyte(SSBE)was proposed to synergistically address those issues.The strong interaction between polyiodides and the organic phase was demonstrated to limit the shuttle effect of polyiodides.Meanwhile,the hybridization of polar organic solvent in the inorganic phase modulated the bonding structure,as well as the effective weakening of water activity,optimizing the interface during zinc electroplating.As a result,the Zn-I_(2)coin cells performed a capacity retention of nearly 100%after 4000 cycles at 2 mA cm^(-2).And a discharge capacity of 0.6 Ah with no degradation after 180 cycles was achieved in the pouch cell.A photovoltaic energy storage battery was further achieved and displayed a cumulative capacity of 5.85 Ah.The successfully designed energy storage device exhibits the application potential of Zn-I_(2)batteries for stationary energy storage.展开更多
基金partially supported by the National Natural Science Foundation of China(22475035 and 22071021)the Natural Science Foundation of Jilin Province(20240101170JC)。
文摘Zinc-iodine batteries have received significant attention due to their high theoretical capacity and environmental friendliness,but their performance is restricted by the growth of zinc dendrites,the hydrogen evolution reaction,and the shuttling effect of polyiodide ions.In this study,an amidoximefunctionalized hydrogel electrolyte,created by amidoximated porous polymer of intrinsic microporosity(AO-PIM-1)and sodium alginate(Alg),is designed to address the aforementioned problems through synergistically optimizing the interfaces of the zinc anode and iodine cathode.The rigid microporous framework and amidoxime groups of AO-PIM-1 can repel polyiodides and inhibit their shuttle effect.Meanwhile,the polyanionic properties of Alg guide the uniform deposition of Zn^(2+)along the(002)crystal plane through the“egg-box”structure,thus suppressing the formation of dendrites.The AO-PIM-1/Alg electrolyte has a high ionic conductivity(18.6 mS cm^(-1)).The assembled symmetric battery can achieve highly reversible dendrite-free zinc plating/stripping(stably cycling for 2550 h at 1 mA cm^(-2)).The Zn-I_(2) full battery with the AO-PIM-1/Alg electrolyte has a long lifespan of 8700 cycles at 0.5 A g^(-1).The working mechanism of the electrolyte was elucidated through density functional theoretical calculations and molecular dynamics simulations.This study provides a new strategy for the hydrogel electrolyte of ZnI_(2) batteries.
基金National Natural Science Foundation of China,Grant/Award Numbers:52372252,51932011Newly Introduced Scientific Research Start-up Funds for High-tech Talents,Grant/Award Number:DD11409024Fundamental Research Funds for the Central Universities of Central South University,Grant/Award Number:2024ZZTS0642。
文摘Static rechargeable zinc-iodine(Zn-I_(2))batteries are superior in safety,costeffectiveness,and sustainability,giving them great potential for large-scale energy storage applications.However,the shuttle effect of polyiodides on the cathode and the unstable anode/electrolyte interface hinder the development of Zn-I_(2)batteries.Herein,a self-segregated biphasic electrolyte(SSBE)was proposed to synergistically address those issues.The strong interaction between polyiodides and the organic phase was demonstrated to limit the shuttle effect of polyiodides.Meanwhile,the hybridization of polar organic solvent in the inorganic phase modulated the bonding structure,as well as the effective weakening of water activity,optimizing the interface during zinc electroplating.As a result,the Zn-I_(2)coin cells performed a capacity retention of nearly 100%after 4000 cycles at 2 mA cm^(-2).And a discharge capacity of 0.6 Ah with no degradation after 180 cycles was achieved in the pouch cell.A photovoltaic energy storage battery was further achieved and displayed a cumulative capacity of 5.85 Ah.The successfully designed energy storage device exhibits the application potential of Zn-I_(2)batteries for stationary energy storage.