Lithium dendrite growth in solid electrolytes is one of the major obstacles to the commercialization of solid-state batteries based on garnet-type solid electrolytes. Herein, we propose a strategy that can simultaneously resolve both the interface and electronic conductivity issues via a simple one-step procedure that provides multilayer protection at low temperature. We take advantage of the facile chemical conversion reaction, showing the wet-coated SnF 2 particles on the solid electrolyte effectively produces a multifunctional interface composed of LiF and Li−Sn alloy upon contact with lithium. We demonstrate the multifunctional interface enables the remarkably high critical current density up to 2.4 mA cm −2 at 25 °C and the stable galvanostatic cycling for over 1000 h at 0.5 mA cm −2 in the lithium symmetric cell. Moreover, the full cell delivers a robust cycle life of more than 600 cycles at 1.0 mA cm −2 , which is the highest performance at room temperature reported to date.
Lithium-rich layered oxides, despite their potential as high-energy-density cathode materials, are impeded by electrochemical performance deterioration upon anionic redox. Although this deterioration is believed to primarily result from structural disordering, our understanding of how it is triggered and/or occurs remains incomplete. Herein, we propose a theoretical picture that clarifies the irreversible transformation and redox asymmetry of lithium-rich layered oxides by introducing a series of global and local dynamic structural evolution processes involving slab gliding and transition-metal migration. We show that slab gliding plays a key role in trigger/initiating the structural disordering and consequent degradation of the anionic redox reaction. We further reveal that the ‘concerted disordering mechanism’ of slab gliding and transition-metal migration produces spontaneously irreversible/asymmetric lithiation and de-lithiation pathways, causing irreversible structural deterioration and the asymmetry of the anionic redox reaction. Our findings suggest slab gliding as a crucial, yet underexplored, method for achieving a reversible anionic redox reaction.
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