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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
Authors
Kang, J[Kang, Joonhee]Chung, H[Chung, Habin]Doh, C[Doh, Chilhoon]Kang, B[Kang, Byoungwoo]Han, B[Han, Byungchan]
DGIST Authors
Kang, J[Kang, Joonhee]; Han, B[Han, Byungchan]
Issue Date
2015-10-20
Citation
Journal of Power Sources, 293, 11-16
Type
Article
Article Type
Article
Keywords
Ab Initio Molecular DynamicsActivation EnergyAluminumAtomsCalculationsChemical ActivationDensity Functional TheoryDiffusion MechanismDiffusion MechanismsElectrolytesFirst-PrinciplesFirst-Principles CalculationFirst Principles Density Functional Theory (DFT) CalculationsGermaniumIonic Conduction In SolidsIonic ConductivityLi-Ion BatteriesLithiumLithium-Ion BatteriesMolecular DynamicsNudged Elastic Band MethodsSolid-State ElectrolyteSolid Electrolytes
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.
Files:
There are no files associated with this item.
Collection:
Energy Science and EngineeringEnergy Systems Engineering1. Journal Articles


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