Sulfur doped Li1.3 Al0.3 Ti1.7 (PO4 )3 solid electrolytes with enhanced ionic conductivity and a reduced activation energy barrier

Physical Chemistry Chemical Physics : PCCP
Abdulkadir KızılaslanHatem Akbulut

Abstract

Recently, tailored synthesis of solid electrolytes satisfy multiple challenges, i.e. high ionic conductivity and wide (electro)chemical stability window is of great interest. Although both oxide- and sulfide-based solid electrolytes have distinguished merits for meeting such concerns separately, a new solid electrolyte having the excellent aspects of both materials is pursued. Herein, we report the synthesis of a sulfur-doped Li1.3Al0.3Ti1.7(PO4)3 (LATP) solid electrolyte with a NASICON crystal structure that combines elevated ionic conductivity with intrinsic stability against an ambient atmosphere. Sulfur doping was carried out using sulfur-amine chemistry and the system was characterized by XRD, Raman, XPS, ICP-OES, and EDS analyses. Bader charge analysis was carried out with the aid of density functional theory calculations to characterize charge accumulation in the local environment of the bare and sulfur doped LATP structures. Our results indicate that the partial replacement of oxygen with sulfur yields higher ionic conductivity due to the lower electronegativity of sulfur compared to oxygen, which reduces the attraction of lithium ions. The enhanced ionic conductivity of LATP is attributed to a decreased lithium ion dif...Continue Reading

References

Oct 15, 1996·Physical Review. B, Condensed Matter·G Kresse, J Furthmüller
Aug 2, 2011·Nature Materials·Noriaki KamayaAkio Mitsui
Mar 22, 2012·Physical Chemistry Chemical Physics : PCCP·V AravindanS Madhavi
Jan 16, 2014·Physical Chemistry Chemical Physics : PCCP·Moran BalaishYair Ein-Eli

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Methods Mentioned

BETA
X-ray
transmission electron microscopy

Software Mentioned

Vienna Ab initio simulation package ( VASP )
NASICON

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