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- W2901412346 abstract "Inorganic solid-state electrolytes (SSEs) couldreplace flammable liquid electrolytes and improve the safety ofLi-ion batteries. Furthermore, these SSEs could enable metalanodes, providing a significant improvement in cell-level energydensity compared to the state-of-the-art. Recent improvements inthe ionic conductivity of ceramic SSEs have invigorated commercialinterest, prompting investigations into SSE/electrode interfacialproperties. However, these investigations have revealed severalchallenges preventing the widespread adoption of all-solid-stateLi-ion batteries. SSEs experience Li dendrite propagation and shortcircuit above a critical current density, similar to liquidelectrolytes. While the pathways for Li penetration through aceramic SSE such as grain boundaries and surface pores have beenidentified, the Li penetration mechanism is unclear. In addition,most SSEs experience detrimental redox reactions at the Li anodeand 4 V cathode interface. The interfacial redox behavior ofinorganic SSEs isn't well understood and requires furtherinvestigation. This thesis investigates the Li penetrationmechanism into sulfide-based amorphous and polycrystalline SSEs,and garnet oxide-based single-crystal and polycrystalline SSEs. Italso investigates the electrochemical redox behavior ofsulfide-based SSEs. Experimental results show that Li can penetrateinto single crystal SSEs devoid of grain boundaries and surfacepores. Above a critical current density, the mechanical stress at acritically-sized Li-filled flaw tip at the SSE surface can breachthe SSE fracture stress to initiate and propagate a crack throughwhich Li penetrates the SSE, until a short circuit occurs. Anelectrochemo- mechanical model based on the Griffith theory ofbrittle ceramic fracture was developed, which relates the SSEfracture stress to SSE fracture toughness and surface flaw size.Experimental determination of the fracture toughness ofsulfide-based SSEs revealed that these SSEs are compliant yetsignificantly more brittle than oxide-based SSEs. In addition, acyclic-voltammetry based technique was developed to show that asulfide-based SSE electrochemically decomposes to produce aredox-active interphase at the SSE/electrode interface. This isunlike in case of liquid electrolytes which decompose into anelectrochemically irreversible interphase." @default.
- W2901412346 created "2018-11-29" @default.
- W2901412346 creator A5090211537 @default.
- W2901412346 date "2018-01-01" @default.
- W2901412346 modified "2023-09-27" @default.
- W2901412346 title "Electro-chemo-mechanical instabilities at interfaces in al-solid-state lithium-ion batteries" @default.
- W2901412346 hasPublicationYear "2018" @default.
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