Manganese‐Based Spinel Cathodes: A Promising Frontier for Solid‐State Lithium‐Ion Batteries

Dou, Yu [Concordia University, Montreal, QC (Canada)]; Zhou, Shiyuan [Argonne National Laboratory (ANL), Argonne, IL (United States)]; Dawkins, Jeremy I. G. [Concordia University, Montreal, QC (Canada)] (ORCID:0000000195412283); Zaghib, Karim [Concordia University, Montreal, QC (Canada)] (ORCID:0000000242017746); Amine, Khalil [Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)]; Xu, Gui‐Liang [Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)] (ORCID:000000019969883X); Deng, Sixu [Concordia University, Montreal, QC (Canada)] (ORCID:0000000174580296)

doi:10.1002/adma.202514126

DOE OSTI · 3374613

Manganese‐Based Spinel Cathodes: A Promising Frontier for Solid‐State Lithium‐Ion Batteries

Dou, Yu [Concordia University, Montreal, QC (Canada)]·Zhou, Shiyuan [Argonne National Laboratory (ANL), Argonne, IL (United States)]·Dawkins, Jeremy I. G. [Concordia University, Montreal, QC (Canada)] (ORCID:0000000195412283)·Zaghib, Karim [Concordia University, Montreal, QC (Canada)] (ORCID:0000000242017746)·Amine, Khalil [Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)]·Xu, Gui‐Liang [Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)] (ORCID:000000019969883X)·Deng, Sixu [Concordia University, Montreal, QC (Canada)] (ORCID:0000000174580296)

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Abstract

Recently, all-solid-state lithium-ion batteries (ASSLIBs), which exhibit improved safety and enhanced energy density compared to conventional commercialized lithium-ion batteries (LIBs), thereby have garnered extensive research interest. Among the promising cathode candidates, Mn-based spinel cathodes LiMn 2 O 4 (LMO) and LiNi 0.5 Mn 1.5 O 4 (LNMO), with the unique characteristics of low cost, structural stability, and 3D Li-ion diffusion channels, have demonstrated excellent performance in LIBs and presented great potential in ASSLIBs applications. However, several challenges, including structural degradations, poor interfacial contact, large interfacial resistance, and Mn-dissolution/diffusion during the electrochemical cycling, hinder their practical applications and commercialization in the ASSLIBs. Particularly, the high-voltage LNMO cathodes suffer from the challenge of electrochemical incompatibility with most of the solid-state electrolytes (SSEs). Herein, the spinel structure, the electrochemical behavior, and the structural degradation of the LMO/LNMO are explored. The characteristics and recent progress of the mitigating strategies to the challenges of various SSEs, including polymer-, oxide-, composite-, sulfide-, halide-, and LiPON-based SSEs, are introduced when paired with LMO/LNMO. Finally, the directions for future research to advance Mn-based spinel cathodes and fulfill the requirements of the next-generation ASSLIBs are also discussed.

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Dou, Yu [Concordia University, Montreal, QC (Canada)], Zhou, Shiyuan [Argonne National Laboratory (ANL), Argonne, IL (United States)], Dawkins, Jeremy I. G. [Concordia University, Montreal, QC (Canada)] (ORCID:0000000195412283), Zaghib, Karim [Concordia University, Montreal, QC (Canada)] (ORCID:0000000242017746), Amine, Khalil [Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)], Xu, Gui‐Liang [Argonne National Laboratory (ANL), Argonne, IL (United States); University of Chicago, IL (United States)] (ORCID:000000019969883X), Deng, Sixu [Concordia University, Montreal, QC (Canada)] (ORCID:0000000174580296). 2025-10-24. Manganese‐Based Spinel Cathodes: A Promising Frontier for Solid‐State Lithium‐Ion Batteries. https://doi.org/10.1002/adma.202514126

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