TY  - JOUR
AU  - Taoussi, S.
AU  - Ouaha, A.
AU  - Naji, M.
AU  - Hoummada, K.
AU  - Lahmar, A.
AU  - Manoun, B.
AU  - El bouari, A.
AU  - frielinghaus, H.
AU  - Zhang, Y.
AU  - Bih, L.
TI  - Novel Zn-doped Nasicon-based glass-ceramic with superior Li-conductivity and enhanced properties as a solid electrolyte
JO  - Acta materialia
VL  - 298
SN  - 1359-6454
CY  - Amsterdam [u.a.]
PB  - Elsevier Science
M1  - FZJ-2025-03307
SP  - 121374 -
PY  - 2025
AB  - Among the diverse array of solid electrolyte options, glass-ceramics hold great promise for application in all-solid-state lithium batteries. In this respect, we have effectively developed novel glasses and glass-ceramics through an innovative approach that integrates a glass-ceramic strategy with the newly introduced zinc-doped Nasicon phase. This was achieved by applying melt-quenching techniques coupled with meticulous control over the crystallization process, guided by a thorough study of crystallization kinetics. The crystallization kinetics have unveiled a two-dimensional nucleation mechanism with an activation energy of 165 kJ.mol-1. X-ray diffraction (XRD) analysis revealed the emergence of a novel Zn-doped Nasicon phase, identified as Li1.6Zn0.3Ti1.7(PO4)3, within the 30Li2O-20ZnO-20TiO2-30P2O5 glass-ceramic, a validation corroborated through Rietveld refinement. Indeed, FT-IR, Raman, and NMR analyses confirmed the formation of Li1+2xZnxTi2-x(PO4)3 Nasicon phase within the glass-ceramics structures. Moreover, SEM images, complemented by TEM observations and density assessments, provide evidence for the creation of a dense, pore-free glass-ceramic with a striped microstructure. The 30Li2O-20ZnO-20TiO2-30P2O5 glass-ceramic demonstrates outstanding chemical durability and robust mechanical properties. Notably, it exhibits high total ionic conductivity, reaching 7.14.10-4 Ω-1.cm-1 at room temperature, while displaying low electronic conductivity of 8.10-9 Ω-1.cm-1, aligning with findings from UV-visible spectroscopy. Additionally, the lithium transference number is confirmed to be 0.99, positioning the developed glass-ceramic as a highly competitive solid electrolyte in the field of energy storage. DFT calculations were conducted on the crystallized Li1.6Zn0.3Ti1.7(PO4)3 NASICON phase to gain detailed insights into its thermodynamic stability and electronic properties.
LB  - PUB:(DE-HGF)16
DO  - DOI:10.1016/j.actamat.2025.121374
UR  - https://juser.fz-juelich.de/record/1044643
ER  -