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DOE OSTI · 2574874

Advancing Mn-Based Li-Ion Battery Cathodes via a Partially Cation-Disordered Zigzag-Type Li–Nb–Mn–O Framework

Wang, You [University of New Mexico, Albuquerque, NM (United States)]·Choe, Wonu [University of New Mexico, Albuquerque, NM (United States)]·Ding, Yong [Georgia Institute of Technology, Atlanta, GA (United States)]·Liu, Rui [University of New Mexico, Albuquerque, NM (United States)]·Nordlund, Dennis [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)]·Chen, Dongchang [University of New Mexico, Albuquerque, NM (United States)] (ORCID:0000000226548176)
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Abstract

Mn-based Li-ion battery cathodes encompass a great variety of materials structures. Decades of research effort have proven that developing a Mn-based structure featuring a high redox activity, stable cycling, and cost-effectiveness is a longstanding challenge. Motivated by such a need and inspired by the structural diversity of Mn-based cathodes, we develop a partially cation-disordered lithium niobium manganese oxide with a zigzag structure, filling the knowledge gap between zigzag-ordered and fully disordered Li-Mn-based oxides. Electrochemically, the partially disordered cathode greatly unlocks the redox activity of the zigzag lattice and maintains the cycling stability. Mechanism-wise, the partial disordering suppresses the disproportionation reaction of Mn(III) and facilitates a disordered λ-MnO 2 -tetragonal cation-disordered rock salt structural transformation. Furthermore, the work suggests the substantial opportunity of using partial disordering as the key strategy to revive locked-up redox activities and realize new energy storage mechanisms, for the pursuit of high-performance cost-effective battery materials.

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25 ENERGY STORAGEChemical structureDiffractionRedox reactionsSpinelTransition metals

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Wang, You [University of New Mexico, Albuquerque, NM (United States)], Choe, Wonu [University of New Mexico, Albuquerque, NM (United States)], Ding, Yong [Georgia Institute of Technology, Atlanta, GA (United States)], Liu, Rui [University of New Mexico, Albuquerque, NM (United States)], Nordlund, Dennis [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)], Chen, Dongchang [University of New Mexico, Albuquerque, NM (United States)] (ORCID:0000000226548176). 2025-04-09. Advancing Mn-Based Li-Ion Battery Cathodes via a Partially Cation-Disordered Zigzag-Type Li–Nb–Mn–O Framework. https://doi.org/10.1021/jacs.5c00139

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