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1. In Situ Formation of Polymer-Inorganic Solid-Electrolyte Interphase for Stable Polymeric Solid-State Lithium Metal Batteries

   https://doi.org/10.1016/j.chempr.2021.06.019  

   Deng, Tao; Cao, Longsheng; He, Xinzi; Li, Ai-Min; Li, Dan; Xu, Jijian; Liu, Sufu; Bai, Panxing; Jin, Ting; Ma, Lin; et al (January 2021, Chem)

   null (Ed.)

   Composite polymer electrolytes (CPEs) for solid-state Li metal batteries (SSLBs) still suffer from gradually increased interface resistance and unconstrained Li dendrite growth. Herein, we addressed the challenges by designing a LiF-rich inorganic solid-electrolyte interphase (SEI) through introducing a fluoride-salt concentrated interlayer on CPE film. The rigid and flexible CPE helps accommodate the volume change of electrodes, while the polymeric high-concentrated electrolyte (PHCE) surface-layer regulates Li-ion flux due to the formation of a stable LiF-rich SEI via anion reduction. The designed CPE-PHCE presents enhanced ionic conductivity and high oxidation stability of > 5.0V (vs. Li/Li+). What’s more, it dramatically reduces the interfacial resistance and achieves a high critical current density of 4.5 mA cm-2 for dendrite-free cycling. The SSLBs, fabricated with thin CPE-PHCE membrane (< 100 μm) and Co-free LiNiO2 cathode, exhibit exceptional electrochemical performance and long cycling stability. This approach of SEI design can also be applied to other types of batteries. 

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2. Solid-state rigid-rod polymer composite electrolytes with nanocrystalline lithium ion pathways

   https://doi.org/10.1038/s41563-021-00995-4  

   Wang, Ying; Zanelotti, Curt J.; Wang, Xiaoen; Kerr, Robert; Jin, Liyu; Kan, Wang Hay; Dingemans, Theo J.; Forsyth, Maria; Madsen, Louis A. (May 2021, Nature Materials)

   Dusastre, Vincent (Ed.)

   A critical challenge for next-generation lithium-based batteries lies in development of electrolytes that enable thermal safety along with use of high-energy-density electrodes. We describe molecular ionic composite (MIC) electrolytes based on an aligned liquid crystalline polymer combined with ionic liquids and concentrated Li salt. This high strength (200 MPa) and non-flammable solid electrolyte possesses outstanding Li+ conductivity (1 mS·cm-1 at 25 °C) and electrochemical stability (5.6 V vs Li|Li+) while suppressing dendrite growth and exhibiting low interfacial resistance (32 Ω·cm2) and overpotentials (≤ 120 mV @ 1 mA·cm-2) during Li symmetric cell cycling. A heterogeneous salt doping process modifies a locally ordered polymer-ion assembly to incorporate an inter-grain network filled with defective LiFSI & LiBF4 nanocrystals, strongly enhancing Li+ conduction. This modular material fabrication platform shows promise for safe and high-energy-density energy storage and conversion applications, incorporating the fast transport of ceramic-like conductors with the superior flexibility of polymer electrolytes. 

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3. Organic–inorganic hybrid electrolytes from ionic liquid-functionalized octasilsesquioxane for lithium metal batteries

   https://doi.org/10.1039/C7TA04599A  

   Yang, Guang; Chanthad, Chalathorn; Oh, Hyukkeun; Ayhan, Ismail Alperen; Wang, Qing (January 2017, Journal of Materials Chemistry A)

   The use of highly conductive solid-state electrolytes to replace conventional liquid organic electrolytes enables radical improvements in the reliability, safety and performance of lithium batteries. Here, we report the synthesis and characterization of a new class of nonflammable solid electrolytes based on the grafting of ionic liquids onto octa-silsesquioxane. The electrolyte exhibits outstanding room-temperature ionic conductivity (∼4.8 × 10 −4 S cm −1 ), excellent electrochemical stability (up to 5 V relative to Li + /Li) and high thermal stability. All-solid-state Li metal batteries using the prepared electrolyte membrane are successfully cycled with high coulombic efficiencies at ambient temperature. The good cycling stability of the electrolyte against lithium has been demonstrated. This work provides a new platform for the development of solid polymer electrolytes for application in room-temperature lithium batteries. 

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4. Ionic Covalent Organic Framework Solid‐State Electrolytes

   https://doi.org/10.1002/adma.202407761  

   Kim, Yoonseob; Li, Chen; Huang, Jun; Yuan, Yufei; Tian, Ye; Zhang, Wei (August 2024, Advanced Materials)

   Rechargeable secondary batteries, widely used in modern technology, are essential for mobile and consumer electronic devices and energy storage applications. Lithium (Li)‐ion batteries are currently the most popular choice due to their decent energy density. However, the increasing demand for higher energy density has led to the development of Li metal batteries (LMBs). Despite their potential, the commonly used liquid electrolyte‐based LMBs present serious safety concerns, such as dendrite growth and the risk of fire and explosion. To address these issues, using solid‐state electrolytes in batteries has emerged as a promising solution. In this Perspective, recent advancements are discussed in ionic covalent organic framework (ICOFs)‐based solid‐state electrolytes, identify current challenges in the field, and propose future research directions. Highly crystalline ion conductors with polymeric versatility show promise as the next‐generation solid‐state electrolytes. Specifically, the use of anionic or cationic COFs is examined for Li‐based batteries, highlight the high interfacial resistance caused by the intrinsic brittleness of crystalline ICOFs as the main limitation, and presents innovative ideas for developing all‐ and quasi‐solid‐state batteries using ICOF‐based solid‐state electrolytes. With these considerations and further developments, the potential for ICOFs is optimistic about enabling the realization of high‐energy‐density all‐solid‐state LMBs. 

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5. High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

   https://doi.org/10.1073/pnas.1907507116  

   Xu, Henghui; Chien, Po-Hsiu; Shi, Jianjian; Li, Yutao; Wu, Nan; Liu, Yuanyue; Hu, Yan-Yan; Goodenough, John B. (September 2019, Proceedings of the National Academy of Sciences)

   Flexible and low-cost poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state Li-metal batteries because of their compatibility with a metallic lithium anode. However, the low room-temperature Li-ion conductivity of PEO solid electrolytes and severe lithium-dendrite growth limit their application in high-energy Li-metal batteries. Here we prepared a PEO/perovskite Li 3/8 Sr 7/16 Ta 3/4 Zr 1/4 O 3 composite electrolyte with a Li-ion conductivity of 5.4 × 10 −5 and 3.5 × 10 −4 S cm −1 at 25 and 45 °C, respectively; the strong interaction between the F − of TFSI − (bis-trifluoromethanesulfonimide) and the surface Ta 5+ of the perovskite improves the Li-ion transport at the PEO/perovskite interface. A symmetric Li/composite electrolyte/Li cell shows an excellent cyclability at a high current density up to 0.6 mA cm −2 . A solid electrolyte interphase layer formed in situ between the metallic lithium anode and the composite electrolyte suppresses lithium-dendrite formation and growth. All-solid-state Li|LiFePO 4 and high-voltage Li|LiNi 0.8 Mn 0.1 Co 0.1 O 2 batteries with the composite electrolyte have an impressive performance with high Coulombic efficiencies, small overpotentials, and good cycling stability. 

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