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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. 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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3. 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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4. Cathodically deposited ZIF-8 compact layer on an 8-µm ultrathin polypropylene separator to enhance the performance of lithium-sulfur and lithium-metal batteries

   https://doi.org/10.1016/j.cej.2024.157192  

   Lin, Xueyan; Baranwal, Rishav; Ren, Guofeng; Fan, Zhaoyang (November 2024, Chemical Engineering Journal)

   The development of high-performance battery technologies necessitates ultrathin separators with superior mechanical strength and electrochemical properties. We present an innovative 1 µm thick, pinhole-free zeolitic imidazolate framework-8 (ZIF-8) layer, cathodically deposited on an 8 µm thick commercial polypropylene (PP) film in a rapid process, resulting in a ZIF-8@8-µm PP flexible membrane. This crack-free ZIF-8 layer, featuring angstrom-scale pores and chemical polar groups, functions as a Li+ sieve, regulating Li+ transport, controlling Li deposition, and blocking dissolved active cathode materials. It also enhances Li+ diffusion and transference number, extending the Sand’s time for Li dendrite formation. Consequently, the ZIF-8@8-µm PP separator addresses polysulfide shuttling in Li-S batteries and Li dendrite formation in Li-metal batteries, significantly improving their performance compared to conventional separators. Our findings indicate that while the 8-μm PP alone is unsuitable as a battery separator, the ZIF-8@8-μm PP, possesses the mechanical strength and electrochemical properties necessary for developing both Li-S and Li-metal batteries, as well as application in conventional Li-ion batteries with enhanced volumetric energy densities. 

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5. Polymer Precursor Derived LixPON Electrolytes: Toward Li−S Batteries

   https://doi.org/https://dx.doi.org/10.1021/acsami.0c03341  

   Temeche, E.; Zhang, X.; Laine, R. M. (April 2020, ACS applied materials interfaces)

   Efforts to develop polymer precursor electrolytes that offer properties anticipated to be similar or superior to (lithium phosphorus oxynitride, LiPON) glasses are reported. Such precursors offer the potential to be used to process LiPON-like thin glass/ceramic coatings for use in all solid state batteries, ASBs. Here, LiPON glasses provide a design basis for the synthesis of sets of oligomers/polymers by lithiation of OP(NH2)3−x(NH)x [from OP(NH)3],OP-(NH2)3‑x(NHSiMe3)x and [PN]3(NHSiMe3)6−x(NH)x. The resulting systems have degrees of polymerization of 5−20. Treatment with selected amounts of LiNH2 provides varying degrees of lithiation and Li+ conducting properties commensurate with Li+ content. Polymer electrolytes impregnated in/on Celgard exhibit Li+ conductivities up to ∼1 × 10−5S cm−1 at room temperature and are thermally stable to ∼150 °C. A Li−S battery assembled using a Li6SiPON composition polymer electrolyte exhibits an initial reversible capacity of 1500 mAhgsulfur −1 and excellent cycle performance at 0.25 and 0.5 C rate over 120 cycles at room temperature. 

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