Tailoring P2/P3‐Intergrowth in Manganese‐Based Layered Transition Metal Oxide Positive Electrodes via Sodium Content for Na‐Ion Batteries

Graff, Kincaid; Hou, Dewen; Gabriel, Eric; Park, Jehee; Koisch, Alex; Schrock, Riley; Conrado, Angel; Schwartz, Darin; Gutierrez, Arturo; Johnson, Christopher S.; Lee, Eungje; Xiong, Hui

doi:10.1002/celc.202400662

Title: Tailoring P2/P3‐Intergrowth in Manganese‐Based Layered Transition Metal Oxide Positive Electrodes via Sodium Content for Na‐Ion Batteries

Journal Article · 05 February 2025 · ChemElectroChem

DOI: https://doi.org/10.1002/celc.202400662 · OSTI ID:2514535

Graff, Kincaid ^[1]; Hou, Dewen ^[1]; Gabriel, Eric ^[1]; Park, Jehee ^[2]; Koisch, Alex ^[1]; Schrock, Riley ^[1]; Conrado, Angel ^[1]; Schwartz, Darin ^[1]; Gutierrez, Arturo ^[2]; Johnson, Christopher S. ^[2]; Lee, Eungje ^[2];

^[1]

Boise State Univ., ID (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

High-manganese content sodium-ion positive electrodes have received heightened interest as an alternative to contemporary Li-ion chemistries due to their high abundance, low toxicity, and even geographical distribution. However, these materials typically suffer from poor capacity, unstable cycling performance, and sluggish Na⁺ kinetics. Herein, we explore a manganese-based layered transition metal oxide (Na_xN_0.25Mn_0.75O₂) and show by X-ray diffraction (XRD) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) that careful variation of the sodium content can instigate the formation of a biphasic intergrowth. This intergrown P2/P3 material offered a higher capacity than its monophasic P2 counterpart due to the P3 structure having greater low-voltage Mn^3+/4+ redox. Further, the intergrowth material offers greatly enhanced kinetics and cycling stability when compared to single-phase P3 material, due to the stabilizing nature of the P2 structure, elucidated by galvanostatic intermittent titration technique (GITT) and operando synchrotron X-ray diffraction. These results highlight the beneficial effect that the intergrowth structure has on the electrochemical performance of high-manganese content positive electrode for future sodium-ion batteries.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357; SC0019121

OSTI ID:: 2514535

Journal Information:: ChemElectroChem, Journal Name: ChemElectroChem Journal Issue: 5 Vol. 12; ISSN 2196-0216

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Tailoring P2/P3‐Intergrowth in Manganese‐Based Layered Transition Metal Oxide Positive Electrodes via Sodium Content for Na‐Ion Batteries

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