Lithium Diffusion Pathways in 3R-LixTiS2: A Combined Neutron Diffraction and Computational
Study
Version 2 2016-08-16, 04:23Version 2 2016-08-16, 04:23
Version 1 2016-02-13, 14:38Version 1 2016-02-13, 14:38
Posted on 2015-05-28 - 00:00
Layered lithium transition-metal
sulfides have long been discussed
as early electrode materials for lithium-ion batteries. However, fundamental
knowledge of lithium-ion migration in these solids is still lacking.
In this study, we report on the diffusion dynamics in lithium-deficient
high-temperature polymorphs of lithium titanium sulfides (3R-LixTiS2; x = 0.7,
0.9) as analyzed using powder neutron diffractometry and density functional
theory (DFT) climbing-image nudged-elastic-band (cNEB) calculations.
Two classes of probable migration pathways have been identified from
the scattering-length density distributions (filtered using the maximum-entropy
method [MEM]) and the probability density functions (PDFs, modeled
from anharmonic Debye–Waller factors): direct diffusion in
the (001) plane as the major mechanism and indirect diffusion through
adjacent tetrahedral voids as a minor mechanism. Calculated activation
barriers agree well with one-particle potentials (OPPs) derived from
measurements for Li0.7TiS2 (0.484[14] and 0.88[4]
eV) but deviate for Li0.9TiS2. The discrepancy
at low defect concentration is attributed to the failure of the OPP
derivation and the different nature of the methods (space-time averaged
vs individual-ion perspective). This work elucidates the pathways
of lithium-ion diffusion in 3R-LixTiS2 and points out pitfalls in established experimental/computational
methods.
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Wiedemann, Dennis; Islam, Mazharul M.; Nakhal, Suliman; Senyshyn, Anatoliy; Bredow, Thomas; Lerch, Martin (2016). Lithium Diffusion Pathways in 3R-LixTiS2: A Combined Neutron Diffraction and Computational
Study. ACS Publications. Collection. https://doi.org/10.1021/acs.jpcc.5b01166