Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state el...Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state electrolytes(PSEs)are competitive candidates for replacing commercial liquid electrolytes due to their flexibility,shape versatility and easy machinability.Despite the rapid development of PSEs,their practical application still faces obstacles including poor ionic conductivity,narrow electrochemical stable window and inferior mechanical strength.Polymer/inorganic composite electrolytes(PIEs)formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes(ISEs),exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics.Some PIEs are highly compatible with high-voltage cathode and lithium metal anode,which offer desirable access to obtaining lithium metal batteries with high energy density.This review elucidates the current issues and recent advances in PIEs.The performance of PIEs was remarkably influenced by the characteristics of the fillers including type,content,morphology,arrangement and surface groups.We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs.Finally,the obstacles and opportunities for creating high-performance PIEs are outlined.This review aims to provide some theoretical guidance and direction for the development of PIEs.展开更多
The lithium dendrite and parasitic reactions are two major challenges for lithium(Li)metal anode—the most promising anode materials for high-energy-density batteries.In this work,both the dendrite and parasitic react...The lithium dendrite and parasitic reactions are two major challenges for lithium(Li)metal anode—the most promising anode materials for high-energy-density batteries.In this work,both the dendrite and parasitic reactions that occurred between the liquid electrolyte and Li-metal anode could be largely inhibited by regulating the Li+-solvation structure.The saturated Li+-solvation species exist in commonly used LiPF 6 liquid electrolyte that needs extra energy to desolvation during Li-electrodeposition.Partial solvation induced high-energy state Li-ions would be more energy favorable during the electron-reduction process,dominating the competition with solvent reduction reactions.The Li-symmetric cells that are cycling at higher temperatures show better performance;the cycled lithium metal anode with metallic lustre and the dendrite-free surface is observed.Theoretical calculation and experimental measurements reveal the existence of high-energy state Li+-solvates species,and their concentration increases with temperature.This study provides insight into the Li+-solvation structure and its electrodeposition characteristics.展开更多
基金the National Natural Science Foundation of China(Nos.22279070,U21A20170 and 22175106)the Ministry of Science and Technology of China(Nos.2019YFA0705703,2021YFB2501900 and 2019YFE0100200)+1 种基金the Tsinghua University Initiative Scientific Research Program(20223080001)the Tsinghua-Foshan Innovation Special Fund(2021THFS0216)。
文摘Solid-state electrolytes(SSEs)are widely considered the essential components for upcoming rechargeable lithium-ion batteries owing to the potential for great safety and energy density.Among them,polymer solid-state electrolytes(PSEs)are competitive candidates for replacing commercial liquid electrolytes due to their flexibility,shape versatility and easy machinability.Despite the rapid development of PSEs,their practical application still faces obstacles including poor ionic conductivity,narrow electrochemical stable window and inferior mechanical strength.Polymer/inorganic composite electrolytes(PIEs)formed by adding ceramic fillers in PSEs merge the benefits of PSEs and inorganic solid-state electrolytes(ISEs),exhibiting appreciable comprehensive properties due to the abundant interfaces with unique characteristics.Some PIEs are highly compatible with high-voltage cathode and lithium metal anode,which offer desirable access to obtaining lithium metal batteries with high energy density.This review elucidates the current issues and recent advances in PIEs.The performance of PIEs was remarkably influenced by the characteristics of the fillers including type,content,morphology,arrangement and surface groups.We focus on the molecular interaction between different components in the composite environment for designing high-performance PIEs.Finally,the obstacles and opportunities for creating high-performance PIEs are outlined.This review aims to provide some theoretical guidance and direction for the development of PIEs.
基金This work was funded by the National Natural Science Foundation of China (52073161 and U1564205)the Ministry of Science and Technology of China (No.2019YFE0100200 and 2019YFA0705703)+1 种基金The authors also thank Joint Work Plan for Research Projects under the Clean Vehicles Consortium at U.S.and China-Clean Energy Research Center (CERC-CVC2.0,2016-2020)thank Tsinghua University-Zhangjiagang Joint Institute for Hydrogen Energy and Lithium Ion Battery Technology.
文摘The lithium dendrite and parasitic reactions are two major challenges for lithium(Li)metal anode—the most promising anode materials for high-energy-density batteries.In this work,both the dendrite and parasitic reactions that occurred between the liquid electrolyte and Li-metal anode could be largely inhibited by regulating the Li+-solvation structure.The saturated Li+-solvation species exist in commonly used LiPF 6 liquid electrolyte that needs extra energy to desolvation during Li-electrodeposition.Partial solvation induced high-energy state Li-ions would be more energy favorable during the electron-reduction process,dominating the competition with solvent reduction reactions.The Li-symmetric cells that are cycling at higher temperatures show better performance;the cycled lithium metal anode with metallic lustre and the dendrite-free surface is observed.Theoretical calculation and experimental measurements reveal the existence of high-energy state Li+-solvates species,and their concentration increases with temperature.This study provides insight into the Li+-solvation structure and its electrodeposition characteristics.
