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| Home > Publications database > Understanding the Electrochemical Reaction Mechanism of the Co/Ni Free Layered Cathode Material P2–Na$_{2/3}$Mn$_{7/12}$Fe$_{1/3}$Ti$_{1/12}$O$_2$ for Sodium-Ion Batteries |
| Journal Article | PUBDB-2024-05802 |
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2024
American Chemical Society
Washington, DC
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Please use a persistent id in citations: doi:10.1021/acs.chemmater.3c01552 doi:10.3204/PUBDB-2024-05802
Abstract: Iron- and manganese-based layered electrodes for sodium-ion batteries have attracted renewed interest due to their low cost and environmental friendliness. However, phase changes at high voltage and the Jahn–Teller effect lead to a short cycle life and poor rate capability. Herein, we describe the optimization of the structure of a Co/Ni free Na$_{2/3}$Mn$_{1/12}$Fe$_{1/12}$O$_2$ cathode via partial substitution of Fe by Mn and Ti and explore the redox activity of P2-type Mn/Fe-based layered cathodes. The obtained P2–Na$_{2/3}$Mn$_{7/12}$Fe$_{1/3}$Ti$_{1/12}$O$_2$ (NMFTO) exhibits a solid solution mechanism during the complete desodiation/resodiation process and delivers an initial discharge capacity of 170 mA h g–1 at a 0.1 C rate and a capacity retention of 80% after 50 cycles. The main focus is to understand the electrochemical mechanism of P2–Na$_{2/3}$Mn$_{7/12}$Fe$_{1/3}$Ti$_{1/12}$O$_2$ by exploring the redox processes of transition metal cations and oxygen anions upon cycling. In situ synchrotron radiation diffraction reveals a single-phase reaction of NMFTO during cycling, which is beneficial to improving cycle stability. In situ X-ray absorption spectroscopy (XAS), in situ 57Fe Mössbauer spectroscopy, and ex situ $^{23}$Na nuclear magnetic resonance spectroscopy are used to elucidate the changes in the crystallographic/electronic structure during desodiation/resodiation. Ex situ soft XAS reveals the participation of oxygen anions in the electrochemical reactions.
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