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1. A room temperature rechargeable Li ₂ O-based lithium-air battery enabled by a solid electrolyte

   https://doi.org/10.1126/science.abq1347  

   Kondori, Alireza; Esmaeilirad, Mohammadreza; Harzandi, Ahmad Mosen; Amine, Rachid; Saray, Mahmoud Tamadoni; Yu, Lei; Liu, Tongchao; Wen, Jianguo; Shan, Nannan; Wang, Hsien-Hau; et al (February 2023, Science)

   A lithium-air battery based on lithium oxide (Li₂O) formation can theoretically deliver an energy density that is comparable to that of gasoline. Lithium oxide formation involves a four-electron reaction that is more difficult to achieve than the one- and two-electron reaction processes that result in lithium superoxide (LiO₂) and lithium peroxide (Li₂O₂), respectively. By using a composite polymer electrolyte based on Li₁₀GeP₂S₁₂nanoparticles embedded in a modified polyethylene oxide polymer matrix, we found that Li₂O is the main product in a room temperature solid-state lithium-air battery. The battery is rechargeable for 1000 cycles with a low polarization gap and can operate at high rates. The four-electron reaction is enabled by a mixed ion–electron-conducting discharge product and its interface with air. 

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2. Crystal structures of sodium-, lithium-, and ammonium 4,5-dihydroxybenzene-1,3-disulfonate (tiron) hydrates

   https://doi.org/10.1107/S2056989018008009  

   Herbst-Gervasoni, Corey J.; Gau, Michael R.; Zdilla, Michael J.; Valentine, Ann M. (July 2018, Acta Crystallographica Section E Crystallographic Communications)

   The solid-state structures of the Na + , Li + , and NH 4 + salts of the 4,5-dihydroxybenzene-1,3-disulfonate (tiron) dianion are reported, namely disodium 4,5-dihydroxybenzene-1,3-disulfonate, 2Na + ·C 6 H 4 O 8 S 2 2− , μ-4,5-dihydroxybenzene-1,3-disulfonato-bis[aqualithium(I)] hemihydrate, [Li 2 (C 6 H 4 O 8 S 2 )(H 2 O) 2 ]·0.5H 2 O, and diammonium 4,5-dihydroxybenzene-1,3-disulfonate monohydrate, 2NH 4 + ·C 6 H 4 O 8 S 2 2− ·H 2 O. Intermolecular interactions vary with the size of the cation, and the asymmetric unit cell, and the macromolecular features are also affected. The sodium in Na 2 (tiron) is coordinated in a distorted octahedral environment through the sulfonate oxygen and hydroxyl oxygen donors on tiron, as well as an interstitial water molecule. Lithium, with its smaller ionic radius, is coordinated in a distorted tetrahedral environment by sulfonic and phenolic O atoms, as well as water in Li 2 (tiron). The surrounding tiron anions coordinating to sodium or lithium in Na 2 (tiron) and Li 2 (tiron), respectively, result in a three-dimensional network held together by the coordinate bonds to the alkali metal cations. The formation of such a three-dimensional network for tiron salts is relatively rare and has not been observed with monovalent cations. Finally, (NH 4 ) 2 (tiron) exhibits extensive hydrogen-bonding arrays between NH 4 + and the surrounding tiron anions and interstitial water molecules. This series of structures may be valuable for understanding charge transfer in a putative solid-state fuel cell utilizing tiron. 

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3. Regulating Li‐Ion Transport through Ultrathin Molecular Membrane to Enable High‐Performance All‐Solid‐State–Battery

   https://doi.org/10.1002/smll.202303625  

   Rajendran, Sathish; George, Antony; Tang, Zian; Neumann, Christof; Turchanin, Andrey; Arava, Leela Mohana (November 2023, Small)

   Abstract Solid‐state lithium metal batteries with garnet‐type electrolyte provide several advantages over conventional lithium‐ion batteries, especially for safety and energy density. However, a few grand challenges such as the propagation of Li dendrites, poor interfacial contact between the solid electrolyte and the electrodes, and formation of lithium carbonate during ambient exposure over the solid‐state electrolyte prevent the viability of such batteries. Herein, an ultrathin sub‐nanometer porous carbon nanomembrane (CNM) is employed on the surface of solid‐state electrolyte (SSE) that increases the adhesion of SSE with electrodes, prevents lithium carbonate formation over the surface, regulates the flow of Li‐ions, and blocks any electronic leakage. The sub‐nanometer scale pores in CNM allow rapid permeation of Li‐ions across the electrode–electrolyte interface without the presence of any liquid medium. Additionally, CNM suppresses the propagation of Li dendrites by over sevenfold up to a current density of 0.7 mA cm⁻²and enables the cycling of all‐solid‐state batteries at low stack pressure of 2 MPa using LiFePO₄cathode and Li metal anode. The CNM provides chemical stability to the solid electrolyte for over 4 weeks of ambient exposure with less than a 4% increase in surface impurities. 

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4. 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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5. Lithium-compatible and air-stable vacancy-rich Li ₉ N ₂ Cl ₃ for high–areal capacity, long-cycling all–solid-state lithium metal batteries

   https://doi.org/10.1126/sciadv.adh4626  

   Li, Weihan; Li, Minsi; Chien, Po-Hsiu; Wang, Shuo; Yu, Chuang; King, Graham; Hu, Yongfeng; Xiao, Qunfeng; Shakouri, Mohsen; Feng, Renfei; et al (October 2023, Science Advances)

   Attaining substantial areal capacity (>3 mAh/cm²) and extended cycle longevity in all–solid-state lithium metal batteries necessitates the implementation of solid-state electrolytes (SSEs) capable of withstanding elevated critical current densities and capacities. In this study, we report a high-performing vacancy-rich Li₉N₂Cl₃SSE demonstrating excellent lithium compatibility and atmospheric stability and enabling high–areal capacity, long-lasting all–solid-state lithium metal batteries. The Li₉N₂Cl₃facilitates efficient lithium-ion transport due to its disordered lattice structure and presence of vacancies. Notably, it resists dendrite formation at 10 mA/cm²and 10 mAh/cm²due to its intrinsic lithium metal stability. Furthermore, it exhibits robust dry-air stability. Incorporating this SSE in Ni-rich LiNi_0.83Co_0.11Mn_0.06O₂cathode-based all–solid-state batteries, we achieve substantial cycling stability (90.35% capacity retention over 1500 cycles at 0.5 C) and high areal capacity (4.8 mAh/cm²in pouch cells). These findings pave the way for lithium metal batteries to meet electric vehicle performance demands. 

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