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Zirconia-based lithium garnet solid electrolytes have attracted much attention in solid-state battery research in recent times due to their high lithium ion conductivity, exceptional stability against lithium metal, and broad electrochemical voltage window. However, the application of these electrolytes for realization of all-solid-state lithium metal batteries has been hindered by large electrode–electrolyte interfacial resistance and severe dendrite growth. This is possibly due to the poor wettability of lithium over the garnet solid electrolyte and inhomogeneous lithium deposition across the metallic lithium|electrolyte interface. To deal with this, herein, we fabricated a lithium–zinc alloy electrode as an alternative for lithium metal for application in solid-state batteries. A systematic investigation has been carried out to study the effect of the Li–Zn anode on the wettability and interface kinetics with a Li6.28Al0.24La3Zr2O12 (LLZA) solid electrolyte. The cross-sectional scanning electron microscopy (SEM) image of Li–Zn|LLZA shows an intimate contact, and the impedance spectrum displays an interface resistance as low as 7.5 Ω cm2 for the Li0.95Zn0.05|LLZA|Li0.95Zn0.05 symmetric cell. In addition to low interfacial resistance, the Li0.95Zn0.05|LLZA|Li0.95Zn0.05 cell exhibited a high critical current density of 1.1 mA cm–2. The cycling capability of the Li0.95Zn0.05 alloy anode was demonstrated by cycling the symmetric cell for 2200 h at 0.35 mA cm–2 and 300 h at 0.5 mA cm–2 without short circuiting, realizing a very high cumulative capacity of 930 mAh cm–2 with a LLZA-based solid-state battery. The result presented here paves the way for an interface-compatible anode for the realization of lithium metal batteries based on garnet-structured solid electrolytes.

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The next-generation electric vehicle requires superior safety and high-energy-density batteries for better performance. Currently, solid polymer electrolytes provide better safety, high mechanical stability, and a desirable electrode-toelectrolyte interface in lithium-ion batteries compared to those in conventional battery systems. However, the ionic conductivity of solid-state electrolytes remains challenging at room and low operating temperatures. Herein, we report that incorporating a greener calcium hydroxide (CH) based nanofiller derived from natural waste seashells with polymer electrolyte gives a tremendously increased lithium-ion conductivity of 4.12 × 10 −5 S cm −1 at 25 °C. The cross-linked composite polymer electrolyte (CCPE) was prepared with PEO, LiClO 4 salt, greener nanofiller, and cross-linking monomers via the facile ultraviolet (UV) polymerization technique. The photosensitive vinyl groups of diacrylate and the thio groups of the tetrathiol monomer undergo a thiol−ene click reaction to form a highly cross-linked network with homogeneously distributed LiClO 4 and CH nanofiller. The incorporation of 15 wt % of CH greener nanofiller significantly improved the amorphous phase of the composite electrolyte and showed a wide electrochemical window of 5 V. The fine porous structure of CH greener nanofiller incorporated in the solid-state cross-linked network electrolyte channelizes for smooth lithium-ion mobility. The fabricated full cell exhibits good discharge capacity, of 160 mAh g −1 to 150 mAh g −1 at 0.1 C over 50 cycles with a high Coulombic efficiency of 95 % at 60 °C. Naturally derived, cost-effective greener nanofiller from waste seashells acts as a prominent additive to prepare solid-state electrolytes with high stability in lithium metal batteries.

Solid-state batteries have been getting considerable attention in recent times due to the safety issues associated with liquid electrolyte-based batteries. However, most rigid solid electrolytes are vulnerable to mechanical strains, so implementation in a commercial battery needs proper modifications. Polymer-type flexible membranes could overcome the size and fragility. Herein, we propose a straightforward preparation of flexible and thin ceramic polymer electrolyte membranes combined with the advantage of garnet-structured fast lithium-ion conductors (Li6.28Al0.24La3Zr2O12) with polyvinylidene fluoride polymers. An 8:2 ratio of garnet to polymer has been employed to create a free-standing flexible ceramic polymer electrolyte through tape casting. The membrane showed excellent electrochemical performance with good conductivity and thermal–electrochemical stability. A facile way of polymer electrolyte casting over lithium iron phosphate electrode material, which contains 5 wt % garnet material, has been adapted to enhance the electrode–electrolyte contact. The cell has offered significantly notable performance. This way, the benefit of solid-state electrolytes could extend to the large-scale production of solid-state batteries with extended safety.

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