Kirkendall effect-induced uniform stress distribution stabilizes nickel-rich layered oxide cathodes

Nickel-rich layered oxide cathodes promise ultrahigh energy density but is plagued by the mechanical failure of the secondary particle upon (de)lithiation. Existing approaches for alleviating the structural degradation could retard pulverization, yet fail to tune the stress distribution and root out the formation of cracks. Herein, we report...

The lasting impact of formation cycling on the Li-ion kinetics between SEI and the Li-metal anode and its correlation with efficiency

Formation cycling is a critical process aimed at improving the performance of lithium ion (Li-ion) batteries during subsequent use. Achieving highly reversible Li-metal anodes, which would boost battery energy density, is a formidable challenge. Here, formation cycling and its impact on the subsequent cycling are largely unexplored. Through...

Reviving the rock-salt phases in Ni-rich layered cathodes by mechano-electrochemistry in all-solid-state batteries

The rock-salt phase (RSP) formed on the surface of Ni-rich layered cathodes in liquid-electrolyte lithium-ion batteries is conceived to be electrochemically "dead". Here we show massive RSP forms in the interior of LiNi_xMn_yCo_(1−x-y)O₂ (NMC) crystals in sulfide based all solid state batteries (ASSBs)...

A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries

Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li_3-3_xM₁₊_xCl₆ (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are...

Improving Li-ion interfacial transport in hybrid solid electrolytes

The development of commercial solid-state batteries has to date been hindered by the individual limitations of inorganic and organic solid electrolytes, motivating hybrid concepts. However, the room-temperature conductivity of hybrid solid electrolytes is still insufficient to support the required battery performance. A key challenge is to...

Revealing the Impact of Space-Charge Layers on the Li-Ion Transport in All-Solid-State Batteries

The influence of space-charge layers on the ionic charge transport over cathode-solid electrolyte interfaces in all-solid-state batteries remains unclear because of the difficulty to unravel it from other contributions to the ion transport over the interfaces. Here, we reveal the effect of the space-charge layers by systematically tuning the...

Tailoring Li6PS5BR ionic conductivity and understanding of its role in cathode mixtures for high performance all-solid-state Li-S batteries

The ultrafast ionic conductivity of Li ₆ PS ₅ Br, which is higher than 1 mS cm ^-1 at room temperature, makes it an attractive candidate electrolyte for the all-solid-state Li-S battery. A simple synthesis route with an easy scale up process is critical for practical applications. In this work, the highest room...

Facile Synthesis toward the Optimal Structure-Conductivity Characteristics of the Argyrodite Li₆PS₅Cl Solid-State Electrolyte

The high Li-ion conductivity of the argyrodite Li₆PS₅Cl makes it a promising solid electrolyte candidate for all-solid-state Li-ion batteries. For future application, it is essential to identify facile synthesis procedures and to relate the synthesis conditions to the solid electrolyte material performance. Here, a...

Revealing the relation between the structure, Li-ion conductivity and solid state battery performance for the argyrodite Li6PS5Br solid electrolyte

Based on its high Li-ion conductivity, argyrodite Li6PS5Br is a promising solid electrolyte for all-solid-state batteries. However, more understanding is required on the relation between the solid electrolyte conductivity and the solid-state battery performance with the argyrodite structure, crystallinity and particle size that depend on the...

Direct view on the phase evolution in individual LiFePO4 nanoparticles during Li-ion battery cycling

Phase transitions in Li-ion electrode materials during (dis)charge are decisive for battery performance, limiting high-rate capabilities and playing a crucial role in the cycle life of Li-ion batteries. However, the difficulty to probe the phase nucleation and growth in individual grains is hindering fundamental understanding and progress. Here...