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Abstract All-solid-state sodium batteries (ASSSBs) are promising candidates for grid-scale energy storage. However, there are no commercialized ASSSBs yet, in part due to the lack of a low-cost, simple-to-fabricate solid electrolyte (SE) with electrochemical stability towards Na metal. In this work, we report a family of oxysulfide glass SEs (Na 3 PS 4− x O x , where 0 <  x  ≤ 0.60) that not only exhibit the highest critical current density among all Na-ion conducting sulfide-based SEs, but also enable high-performance ambient-temperature sodium-sulfur batteries. By forming bridging oxygen units, the Na 3 PS 4− x O x SEs undergo pressure-induced sintering at room temperature, resulting in a fully homogeneous glass structure with robust mechanical properties. Furthermore, the self-passivating solid electrolyte interphase at the Na|SE interface is critical for interface stabilization and reversible Na plating and stripping. The new structural and compositional design strategies presented here provide a new paradigm in the development of safe, low-cost, energy-dense, and long-lifetime ASSSBs.

Abstract Single-crystalline nickel-rich cathodes are a rising candidate with great potential for high-energy lithium-ion batteries due to their superior structural and chemical robustness in comparison with polycrystalline counterparts. Within the single-crystalline cathode materials, the lattice strain and defects have significant impacts on the intercalation chemistry and, therefore, play a key role in determining the macroscopic electrochemical performance. Guided by our predictive theoretical model, we have systematically evaluated the effectiveness of regaining lost capacity by modulating the lattice deformation via an energy-efficient thermal treatment at different chemical states. We demonstrate that the lattice structure recoverability is highly dependent on both the cathode composition and the state of charge, providing clues to relieving the fatigued cathode crystal for sustainable lithium-ion batteries.

Active particles in composite electrodes initially show asynchronous activity that evolves toward synchronous behavior.

Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) is a promising inorganic solid electrolyte due to its high Li + conductivity and electrochemical stability for all-solid-state batteries. Mechanical characterization of LLZTO is limited by the synthesis of the condensed phase. Here we systematically measure the elastic modules, hardness, and fracture toughness of LLZTO polycrystalline pellets of different densities using the customized environmental nanoindentation. The LLZTO samples are sintered using the hot-pressing method with different amounts of Li 2 CO 3 additives, resulting in the relative density of the pellets varying from 83% to 98% and the largest grain size of 13.21 ± 5.22 μm. The mechanical properties show a monotonic increase as the sintered sample densifies, elastic modulus and hardness reach 158.47 ± 10.10 GPa and 11.27 ± 1.38 GPa, respectively, for LLZTO of 98% density. Similarly, fracture toughness increases from 0.44 to 1.51 MPa⋅m 1/2 , showing a transition from the intergranular to transgranular fracture behavior as the pellet density increases. The ionic conductivity reaches 4.54 × 10 −4 S/cm in the condensed LLZTO which enables a stable Li plating/stripping in a symmetric solid-state cell for over 100 cycles. This study puts forward a quantitative studymore »of the mechanical behavior of LLZTO of different microstructures that is relevant to the mechanical stability and electrochemical performance of all-solid-state batteries.« less