Article Dans Une Revue Ceramics International Année : 2024

Glass-ceramics and molybdenum doping synergistic approach for Nasicon-type solid-state electrolytes

Résumé

Advancing energy density, enabling lithium metal anodes, and ensuring unparalleled safety and operational reliability in lithium batteries hinge on advancing inorganic solid-state electrolytes. To overcome current impediments, we present an innovative approach that integrates glass-ceramics with a pioneering new Nasicon strategy involving molybdenum doping. In the conducted study, a series of 14Li2O-9Al2O3-38TiO2-(39-x)P2O5-xMoO3 glasses, denoted as LATPMox, along with their corresponding glass-ceramics (LATPMox-GC), have exhibited a promising characteristic as solid electrolytes. X-ray diffraction (XRD) analysis confirms the formation of the novel Mo-doped Nasicon phases in the glass-ceramics, as validated by Rietveld refinement. Examination of the crystallization kinetic behavior of the glasses reveals a three-dimensional nucleation process with spherical particle growth, featuring an activation energy of 165 kJ.mol-1. Transmission Electron Microscopy TEM characterization aligns crystallization behavior with crystallite and distribution within the glass matrix, resulting in a compact and dense microstructure. The structural properties of the resultant phases are examined through FT-IR, Raman spectroscopy, and TEM-SEAD analysis. Vickers indentation tests were employed to assess the microscopic fracture toughness, and both the glass and glass-ceramics materials demonstrated favorable mechanical performance. Optical characterization using UV-visible absorption highlights the reduction of Mo6+ to Mo5+, likely occupying tetrahedral sites within the crystalline lattice. Impedance spectroscopy measurement showcases the effective promotion of ionic conductivity following Mo doping, reaching a total conductivity value of 5.50×10-5 Ω-1.cm-1 along with a high lithium transference number of 0.99 at room temperature for LATPMo2.6-GC glass-ceramic. This value is larger than that of many other glass-ceramics as well as that of the well-known lithium phosphorous oxy-nitride LiPON solid electrolyte whose ionic conductivity at RT is around 2×10-6 Ω-1.cm-1.
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Dates et versions

hal-04711260 , version 1 (26-09-2024)

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S. Taoussi, K. Hoummada, A. Lahmar, M. Naji, H. Bih, et al.. Glass-ceramics and molybdenum doping synergistic approach for Nasicon-type solid-state electrolytes. Ceramics International, 2024, ⟨10.1016/j.ceramint.2024.09.255⟩. ⟨hal-04711260⟩
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