Interphase Stabilization of LiNi0.5Mn1.5O4 Cathode for 5 V–Class All–Solid–State Batteries

Lee, Dongsoo; Cui, Zehao; Goodenough, John B.; Manthiram, Arumugam

doi:10.1002/smll.202306053

Title: Interphase Stabilization of LiNi_0.5Mn_1.5O₄ Cathode for 5 V–Class All–Solid–State Batteries

Journal Article · Fri Sep 01 00:00:00 EDT 2023 · Small

DOI:https://doi.org/10.1002/smll.202306053· OSTI ID:2217467

Lee, Dongsoo ^[1]; Cui, Zehao ^[1]; Goodenough, John B. ^[1];

^[1]

University of Texas at Austin, TX (United States)

Abstract Employing high voltage cobalt‐free spinel LiNi _0.5 Mn _1.5 O ₄ (LNMO) as a cathode is promising for high energy density and cost‐effectiveness, but it has challenges in all‐solid‐state batteries (ASSBs). Here, it is revealed that the limitation of lithium argyrodite sulfide solid electrolyte (Li ₆ PS ₅ Cl) with the LNMO cathode is due to the intrinsic chemical incompatibility and poor oxidative stability. Through a careful analysis of the interphase of LNMO, it is elucidated that even the halide solid electrolyte (Li ₃ InCl ₆ ) with high oxidative stability can be decomposed to form resistive interphase layers with LNMO in ASSBs. Interestingly, with Fe‐doping and a Li ₃ PO ₄ protective layer coating, LNMO with Li ₃ InCl ₆ displays stable cycle performance with a stabilized interphase at a high voltage (≈4.7 V) in ASSBs. The enhanced interfacial stability with the extended electrochemical stability window through doping and coating enables high electrochemical stability with LNMO in ASSBs. This work provides guidance for employing high‐voltage cathodes in ASSBs and highlights the importance of stable interphases to enable stable cycling in ASSBs.

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Research Organization:: University of Texas at Austin, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); Welch Foundation; USDOE

Grant/Contract Number:: EE0007762; F-1254; DE‐EE0007762

OSTI ID:: 2217467

Alternate ID(s):: OSTI ID: 2281428

Journal Information:: Small, Vol. 20, Issue 2; ISSN 1613-6810

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
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interface
electrochemistry

Title: Interphase Stabilization of LiNi0.5Mn1.5O4 Cathode for 5 V–Class All–Solid–State Batteries

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Title: Interphase Stabilization of LiNi_0.5Mn_1.5O₄ Cathode for 5 V–Class All–Solid–State Batteries