Journal Article PUBDB-2025-03804

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Insights into the Redox Chemistry and Structural Evolution of a P2-Type Cathode Material in Sodium-Ion Batteries

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2025
American Chemical Society Washington, DC

Chemistry of materials 37(4), 1588 - 1599 () [10.1021/acs.chemmater.4c03201]
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Abstract: In view of the tunable composition and higher theoretical capacity, layered transition metal oxide cathode materials (Na$_x$TMO$_2$, TM: transition metal) have attained substantial attention. In this work, a P2-type layered metal oxide with the nominal composition Na$_{0.67}$Fe$_{0.20}$Ni$_{0.15}$Mn$_{0.65}$O$_2$ (NFNM) was synthesized via a sol–gel method; electrochemical performance and the operating mechanism of the electrode material in half-cells were investigated. The material delivered an initial discharge capacity of 166 mA h g$^{–1}$ where the capacity retention after 50 cycles is 65% when cycled in the voltage range 1.50–4.30 V at a C-rate of C/20. At 1C, the capacity delivered by the material was 110 mA h g$^{–1}$ and the capacity retention noted after 80 cycles was 80%. A combination of in operando synchrotron diffraction and X-ray absorption spectroscopy (XAS) elucidates the electrochemical mechanism in a Na/NFNM half-cell. The structural evolution of the electrode material was analyzed using in operando XRD from which the evidence of reversible P2-Z phase transformations was obtained. Investigation of the charge-compensation mechanism and local structure changes in the electrode material during cycling were carried out via the XAS technique which revealed the coupled Fe migration, anionic activity, and phase transformations.

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Contributing Institute(s):
  1. DOOR-User (DOOR ; HAS-User)
Research Program(s):
  1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
  2. DFG project G:(GEPRIS)390874152 - EXC 2154: POLiS - Post Lithium Storage Cluster of Excellence (390874152) (390874152)
Experiment(s):
  1. PETRA Beamline P65 (PETRA III)

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 Record created 2025-08-26, last modified 2025-09-02


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