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Degradation Pathways of Cobalt-Free LiNiO_2 Cathode in Lithium Batteries

机译：Degradation Pathways of Cobalt-Free LiNiO_2 Cathode in Lithium Batteries

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摘要

Electrode-electrolyte reactivity (EER) and particle cracking (PC) are consideredtwo main causes of capacity fade in high-nickel layered oxide cathodes inlithium-based batteries. However, whether EER or PC is more critical remainsdebatable. Herein, the fundamental correlation between EER and PC is systematicallyinvestigated with LiNiO_2 (LNO), the ultimate cobalt-free lithiumlayered oxide cathode. Specifically, EER is found more critical than secondaryparticle cracking (SPC) in determining the cycling stability of LNO; EER leadsto primary particle cracking, but mitigates SPC due to the inhibition of H2-H3phase transformation. Two surface degradation pathways are identified forcycled LNO under low and high EERs. A common blocking surface reconstructionlayer (SRL) containing electrochemically-inactive Ni_3O_4 spinel andNiO rock-salt phases is formed on LNO in an electrolyte with a high EER; incontrast, an electrochemically-active SRL featuring regions of electron- andlithium-ion-conductive LiNi_2O_4 spinel phase is formed on LNO in an electrolytewith a low EER. These findings unveil the intrinsic degradation pathwaysof LNO cathode and are foreseen to provide new insights into the developmentof lithium-based batteries with a minimized EER and a maximizedservice life.

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