Solid polymer electrolytes(SPEs)are considered to be one of the most promising systems applied in all-solid-state lithium metal batteries(ASSLMBs)on account of their chemical and electrochemical ro bustness,mechanical...Solid polymer electrolytes(SPEs)are considered to be one of the most promising systems applied in all-solid-state lithium metal batteries(ASSLMBs)on account of their chemical and electrochemical ro bustness,mechanical stability,cost-effective and scalable manufacturing techniques.Lately,significant en deavors have been directed towards mitigating the formation of the Li dendrite in SPE-based ASSLMBs while research on the inactive lithium in the forms of the solid-electrolyte interface has been rarely re ported.Herein,a bi-functional GaI3additive is developed for in-situ generating Li_(3)Ga alloy for suppressing Li dendrite growth,as well as I3-in recovering dead lithium.Relying on the density functional theory(DFT)results,the Li atom prefers to deposit on the Li_(3)Ga surface and then guide uniform Li deposi tion,while the I3species features a relatively lower lowest unoccupied molecular orbital(LUMO)energy level(-2.12 e V),meaning a higher electron affinity,which is beneficial for reviving inactive lithium to counterbalance the loss of lithium.As a result,in comparison to cells employing pure PEGDME-based electrolytes,the Li-Li symmetric cells utilizing GaI3-containing solid-state electrolyte exhibited a cycling life nearly 30 times longer at a current density/capacity of 0.2 mA/cm^(2),0.2 mAh/cm^(2).The full batterie of LFP//1%GaI3-SPE//40μm Li delivered a noteworthy capacity retention of 82%after 1300 cycles at a rate of 1 C.展开更多
基金supported by the National Natural Science Foundation of China.(Nos.22208039,51961125207)the Basic Scientific Research Project of the Educational Department of Liaoning Province(No.LJKMZ20220878)+1 种基金the Dalian Science and Technology Talent Innovation Support Plan(No.2022RQ036)the Dalian Polytechnic University(Nos.6102072202,2023044)。
文摘Solid polymer electrolytes(SPEs)are considered to be one of the most promising systems applied in all-solid-state lithium metal batteries(ASSLMBs)on account of their chemical and electrochemical ro bustness,mechanical stability,cost-effective and scalable manufacturing techniques.Lately,significant en deavors have been directed towards mitigating the formation of the Li dendrite in SPE-based ASSLMBs while research on the inactive lithium in the forms of the solid-electrolyte interface has been rarely re ported.Herein,a bi-functional GaI3additive is developed for in-situ generating Li_(3)Ga alloy for suppressing Li dendrite growth,as well as I3-in recovering dead lithium.Relying on the density functional theory(DFT)results,the Li atom prefers to deposit on the Li_(3)Ga surface and then guide uniform Li deposi tion,while the I3species features a relatively lower lowest unoccupied molecular orbital(LUMO)energy level(-2.12 e V),meaning a higher electron affinity,which is beneficial for reviving inactive lithium to counterbalance the loss of lithium.As a result,in comparison to cells employing pure PEGDME-based electrolytes,the Li-Li symmetric cells utilizing GaI3-containing solid-state electrolyte exhibited a cycling life nearly 30 times longer at a current density/capacity of 0.2 mA/cm^(2),0.2 mAh/cm^(2).The full batterie of LFP//1%GaI3-SPE//40μm Li delivered a noteworthy capacity retention of 82%after 1300 cycles at a rate of 1 C.
