Cited 2 time in webofscience Cited 2 time in scopus

First-Principles Characterization of the Unknown Crystal Structure and Ionic Conductivity of Li7P2S8I as a Solid Electrolyte for High-Voltage Li Ion Batteries

Title
First-Principles Characterization of the Unknown Crystal Structure and Ionic Conductivity of Li7P2S8I as a Solid Electrolyte for High-Voltage Li Ion Batteries
Authors
Kang, J[Kang, Joonhee]Han, B[Han, Byungchan]
DGIST Authors
Kang, J[Kang, Joonhee]
Issue Date
2016-07-21
Citation
Journal of Physical Chemistry Letters, 7(14), 2671-2675
Type
Article
Article Type
Article
Keywords
Ab Initio Molecular Dynamics SimulationActivation EnergyAtomic-Level MechanismsAttractive InteractionsCalculationsComputation TheoryComputational DesignConceptual ApproachesCrystal Atomic StructureCrystal StructureDensity Functional TheoryElectric BatteriesElectrochemical InstabilityElectrolytesFirst-Principles Density Functional TheoryIodineIonic ConductivityIonsLithiumLithium-Ion BatteriesMolecular DynamicsSolid ElectrolytesSulfide-Based Solid Electrolytes
ISSN
1948-7185
Abstract
Using first-principles density functional theory calculations and ab initio molecular dynamics (AIMD) simulations, we demonstrate the crystal structure of the Li7P2S8I (LPSI) and Li ionic conductivity at room temperature with its atomic-level mechanism. By successively applying three rigorous conceptual approaches, we identify that the LPSI has a similar symmetry class as Li10GeP2S12 (LGPS) material and estimate the Li ionic conductivity to be 0.3 mS cm-1 with an activation energy of 0.20 eV, similar to the experimental value of 0.63 mS cm-1. Iodine ions provide an additional path for Li ion diffusion, but a strong Li-I attractive interaction degrades the Li ionic transport. Calculated density of states (DOS) for LPSI indicate that electrochemical instability can be substantially improved by incorporating iodine at the Li metallic anode via forming a LiI compound. Our methods propose the computational design concept for a sulfide-based solid electrolyte with heteroatom doping for high-voltage Li ion batteries. © 2016 American Chemical Society.
URI
http://hdl.handle.net/20.500.11750/2235
DOI
10.1021/acs.jpclett.6b01050
Publisher
American Chemical Society
Files:
There are no files associated with this item.
Collection:
Energy Science and EngineeringETC1. Journal Articles


qrcode mendeley

Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.

BROWSE