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About the Compatibility between High Voltage Spinel Cathode Materials and Solid Oxide Electrolytes as a Function of Temperature

  • Author(s): Miara, L
  • Windmüller, A
  • Tsai, CL
  • Richards, WD
  • Ma, Q
  • Uhlenbruck, S
  • Guillon, O
  • Ceder, G
  • et al.

© 2016 American Chemical Society. The reactivity of mixtures of high voltage spinel cathode materials Li2NiMn3O8, Li2FeMn3O8, and LiCoMnO4cosintered with Li1.5Al0.5Ti1.5(PO4)3and Li6.6La3Zr1.6Ta0.4O12electrolytes is studied by thermal analysis using X-ray-diffraction and differential thermoanalysis and thermogravimetry coupled with mass spectrometry. The results are compared with predicted decomposition reactions from first-principles calculations. Decomposition of the mixtures begins at 600 °C, significantly lower than the decomposition temperature of any component, especially the electrolytes. For the cathode + Li6.6La3Zr1.6Ta0.4O12mixtures, lithium and oxygen from the electrolyte react with the cathodes to form highly stable Li2MnO3and then decompose to form stable and often insulating phases such as La2Zr2O7, La2O3, La3TaO7, TiO2, and LaMnO3which are likely to increase the interfacial impedance of a cathode composite. The decomposition reactions are identified with high fidelity by first-principles calculations. For the cathode + Li1.5Al0.5Ti1.5(PO4)3mixtures, the Mn tends to oxidize to MnO2or Mn2O3, supplying lithium to the electrolyte for the formation of Li3PO4and metal phosphates such as AlPO4and LiMPO4(M = Mn, Ni). The results indicate that high temperature cosintering to form dense cathode composites between spinel cathodes and oxide electrolytes will produce high impedance interfacial products, complicating solid state battery manufacturing.

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