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Integrated study of first principles calculations and experimental measurements for Li-ionic conductivity in Al-doped solid-state LiGe2(PO4)(3) electrolyte

Title
Integrated study of first principles calculations and experimental measurements for Li-ionic conductivity in Al-doped solid-state LiGe2(PO4)(3) electrolyte
Author(s)
Kang, JoonheeChung, HabinDoh, ChilhoonKang, ByoungwooHan, Byungchan
Issued Date
2015-10-20
Citation
Journal of Power Sources, v.293, pp.11 - 16
Type
Article
Author Keywords
Li-ion batteriesFirst principlesSolid-state electrolyteIonic conductivityDiffusion mechanism
Keywords
Ab Initio Molecular DynamicsACTIVATIONActivation EnergyAluminumAtomsCalculationsCATHODEChemical ActivationCONDUCTORSDensity Functional TheoryDiffusion MechanismDiffusion MechanismsElectrochemical PropertiesElectrolytesENERGYFirst-Principles CalculationFirst PrinciplesFirst Principles Density Functional Theory (DFT) CalculationsGEGermaniumGLASS-CERAMICSIonic Conduction in SolidsIonic ConductivityLi-Ion BatteriesLithiumLithium-Ion BatteriesLITHIUM BATTERYMolecular DynamicsNudged Elastic Band MethodsPHOSPHATESolid-State ElectrolyteSolid ElectrolytesSTABILITY
ISSN
0378-7753
Abstract
Understanding of the fundamental mechanisms causing significant enhancement of Li-ionic conductivity by Al3+ doping to a solid LiGe2(PO4)3 (LGP) electrolyte is pursued using first principles density functional theory (DFT) calculations combined with experimental measurements. Our results indicate that partial substitution Al3+ for Ge4+ in LiGe2(PO4)3 (LGP) with aliovalent (Li1+xAlxGe2-x(PO4)3, LAGP) improves the Li-ionic conductivity about four-orders of the magnitude. To unveil the atomic origin we calculate plausible diffusion paths of Li in LGP and LAGP materials using DFT calculations and a nudged elastic band method, and discover that LAGP had additional transport paths for Li with activation barriers as low as only 34% of the LGP. Notably, these new atomic channels manifest subtle electrostatic environments facilitating cooperative motions of at least two Li atoms. Ab-initio molecular dynamics predict Li-ionic conductivity for the LAGP system, which is amazingly agreed experimental measurement on in-house made samples. Consequently, we suggest that the excess amounts of Li caused by the aliovalent Al3+ doping to LGP lead to not only enhancing Li concentration but also opening new conducting paths with substantially decreases activation energies and thus high ionic conductivity of LAGP solid-state electrolyte. © 2015 Published by Elsevier B.V.
URI
http://hdl.handle.net/20.500.11750/2830
DOI
10.1016/j.jpowsour.2015.05.060
Publisher
Elsevier B.V.
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Appears in Collections:
Department of Energy Science and Engineering Energy Systems Engineering 1. Journal Articles

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