Journal
JOURNAL OF SOLID STATE ELECTROCHEMISTRY
Volume 16, Issue 5, Pages 1807-1813Publisher
SPRINGER
DOI: 10.1007/s10008-011-1572-8
Keywords
Lithium ion conduction; Bond valence; Ion transport; Neutron diffraction
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Funding
- Singapore Ministry of Education [MOE2009-T2-1-065]
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All-solid-state rechargeable lithium-ion batteries (AS-LIBs) are attractive power sources for electrochemical applications due to their potentiality in improving safety and stability over conventional batteries with liquid electrolytes. Finding a solid electrolyte with high ionic conductivity and compatibility with other battery components is a key factor in raising the performance of AS-LIBs. In this work, we prepare argyrodite-type Li6PS5X (X = Cl, Br, I) using mechanical milling followed by annealing. X-ray diffraction characterization reveals the formation and growth of crystalline Li6PS5X in all cases. Ionic conductivity of the order of 7 x 10(-4) S cm(-1) in Li6PS5Cl and Li6PS5Br renders these phases suitable for AS-LIBs. Joint structure refinements using high-resolution neutron and laboratory X-ray diffraction provide insight into the influence of disorder on the fast ionic conductivity. Besides the disorder in the lithium distribution, it is the disorder in the S2-/Cl- or S2-/Br- distribution that we find to promote ion mobility, whereas the large I- cannot be exchanged for S2- and the resulting more ordered Li6PS5I exhibits only a moderate conductivity. Li+ ion migration pathways in the crystalline compounds are modelled using the bond valence approach to interpret the differences between argyrodites containing different halide ions.
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