Promoting Reversible Anionic Redox in Sodium-Ion Cathodes by Doping and Phase Control

Jia, Shipeng [McGill University, Montreal, QC (Canada)]; Abdolhosseini, Marzieh [McGill University, Montreal, QC (Canada)]; Li, Yixuan [McGill University, Montreal, QC (Canada)]; Lee, Sang-Jun [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000281993993); Ogasawara, Hirohito [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000153381079); Chen, Ning [Canadian Light Source Inc., Saskatoon, SK (Canada)] (ORCID:0000000212696119); Hebert, Alexander [McGill University, Montreal, QC (Canada)]; Sieffert, J. Michael [McGill University, Montreal, QC (Canada)] (ORCID:0000000250690287); Eisnor, Maddison Margaret [McGill University, Montreal, QC (Canada)] (ORCID:0000000296197981); McCalla, Eric [McGill University, Montreal, QC (Canada)] (ORCID:000000020557608X)

doi:10.1021/acsmaterialslett.4c02597

DOE OSTI · 2589366

Promoting Reversible Anionic Redox in Sodium-Ion Cathodes by Doping and Phase Control

Jia, Shipeng [McGill University, Montreal, QC (Canada)]·Abdolhosseini, Marzieh [McGill University, Montreal, QC (Canada)]·Li, Yixuan [McGill University, Montreal, QC (Canada)]·Lee, Sang-Jun [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000281993993)·Ogasawara, Hirohito [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000153381079)·Chen, Ning [Canadian Light Source Inc., Saskatoon, SK (Canada)] (ORCID:0000000212696119)·Hebert, Alexander [McGill University, Montreal, QC (Canada)]·Sieffert, J. Michael [McGill University, Montreal, QC (Canada)] (ORCID:0000000250690287)·Eisnor, Maddison Margaret [McGill University, Montreal, QC (Canada)] (ORCID:0000000296197981)·McCalla, Eric [McGill University, Montreal, QC (Canada)] (ORCID:000000020557608X)

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Abstract

Important efforts are underway to harness anionic redox to obtain high-energy Na-ion cathodes. Previously, we identified disruptive dopants in Na–Mn–O that induced reversible oxygen redox. Here, we perform detailed mechanistic studies to understand why these dopants are effective. First, we confirm that no transition metals (TMs) are being oxidized─it is indeed oxygen redox. We also identify that reversible TM migration occurs in the P2 phase where reversible anionic redox occurs, while the migration is irreversible in the distorted P′2 phase. Structural control over the anionic redox is highly significant, but we further elucidate the role of the disruptive dopants. Localized oxygen holes are identified as the source of the reversible anionic redox, and these are deemed to remain stable due to the dopants minimizing the interactions between oxygens to prevent their dimerization. Furthermore, these important contributions to understanding anionic redox will help realize viable high-energy Na-ion batteries.

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Impurities Materials Oxygen Redox reactions Transition metals

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Jia, Shipeng [McGill University, Montreal, QC (Canada)], Abdolhosseini, Marzieh [McGill University, Montreal, QC (Canada)], Li, Yixuan [McGill University, Montreal, QC (Canada)], Lee, Sang-Jun [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000281993993), Ogasawara, Hirohito [SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)] (ORCID:0000000153381079), Chen, Ning [Canadian Light Source Inc., Saskatoon, SK (Canada)] (ORCID:0000000212696119), Hebert, Alexander [McGill University, Montreal, QC (Canada)], Sieffert, J. Michael [McGill University, Montreal, QC (Canada)] (ORCID:0000000250690287), Eisnor, Maddison Margaret [McGill University, Montreal, QC (Canada)] (ORCID:0000000296197981), McCalla, Eric [McGill University, Montreal, QC (Canada)] (ORCID:000000020557608X). 2025-03-13. Promoting Reversible Anionic Redox in Sodium-Ion Cathodes by Doping and Phase Control. https://doi.org/10.1021/acsmaterialslett.4c02597

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