Insights into structural stability and Li superionic conductivity of Li10GeP2S12 from first-principles calculations

Hu, Cong; Wang, Zhiqiang; Sun, Zhiwei; Ouyang, Chuying

doi:10.1016/j.cplett.2013.11.003

Cited by 39 publications

(18 citation statements)

References 22 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The primitive cell of LGPS has been used for all calculations in the present study. The same choice of cell size has been made in all the earlier studies on LGPS based on DFT. ,,,, The restriction on the size arises majorly due to the exponential nature of the increase in configurational space with cell size. The configurational space within the primitive cell itself is huge ( 32 C 20 , not accounting for the symmetry).…”

Section: Methodsmentioning

confidence: 99%

“…However, the numbers verified the anisotropy and the diffusional preference along the c channel. Further, Hu et al reported the ab initio calculations by including the van der Waals interactions and found a dramatically different result: c channel energy barrier of 0.23–0.27 eV and ab plane energy barrier of 0.11–0.18 eV . According to them, diffusion is dominant along the ab plane, and LGPS is a 3D ionic conductor.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Origin of Fast Ion Conduction in Li₁₀GeP₂S₁₂, a Superionic Conductor

Bhandari

Bhattacharya

2016

J. Phys. Chem. C

View full text Add to dashboard Cite

The discovery of additional sites has revealed important insights into the possibility of cross-channel ionic diffusion in Li10GeP2S12 (LGPS). Here, we present an ab initio study of a Li diffusion mechanism in LGPS. The presence of fractional occupancy for Li sites leads to different c channel population of Li and different local environment for Li hop both along the c-directional channels and in the ab plane. We perform a rigorous computation of the energy barriers with different population of Li and different environment of Li surrounding the c channels. It is found that the diffusion energy barrier in LGPS depends significantly on channel population, local environment, and the type of hop which leads to a range of relative diffusivity along different directions. A novel mechanism of correlated diffusion between the c channel and the ab plane is found with significantly low energy barrier. The relative frequency of occurrence of the novel hop mechanism critically controls the degree of anisotropy in LGPS. Moreover, low activation barrier associated with this hop leads to high diffusivity which is sustained even after repeated cycling due to the presence of cross-channel pathways.

show abstract

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Origin of Fast Ion Conduction in Li₁₀GeP₂S₁₂, a Superionic Conductor

Bhandari

Bhattacharya

2016

J. Phys. Chem. C

View full text Add to dashboard Cite

show abstract

“…Their computational studies were very useful for researchers studying sulfide electrolytes and led to better understanding of the stability of the electrolyte and electrode materials. In addition, Hu et al [ 274 ] and Du et al [ 275 ] performed computational analysis on LGPS-type structures, Binninger et al [ 276 ] investigated the electrochemical stability window of LGPS-type structures, and Gorai et al [ 277 ] performed electronic structure and defect chemistry calculations for LGPS-type structures.…”

Section: Sulfide Solid Electrolytesmentioning

confidence: 99%

“…Li 11−x M 2−x P 1+x S 12 (M = Ge, Sn, Si) (LGPS)-Type StructuresIn 2011, Kamaya et al[266] synthesized the Li 10 GeP 2 S 12 (LGPS) solid electrolyte and reported a conductivity of 9 × 10 -3 S cm −1(Table 1)and electrochemical properties of a LiCoO 2 -LGPS|LGPS|In cell. Moreover, other researchers have extensively analyzed this system[267][268][269][270][271][272][273][274][275][276][277].LGPS presented tetragonal crystal structure with the lattice parameters a = 8.708 Å and c = 12.605 Å and consisted of negatively charged PS4 3− and GeS 4 4− tetrahedra surrounded by (mobile) Li + ions for charge compensation as shown inFigure 17a,and X-ray powder diffraction patterns and Rietveld refinements of Li 11 Si 2 PS 12 and Li 10 SnP 2 S 12 are compared with those previously reported for Li 10 GeP 2 S 12 and Li 7 GePS 8 in…”

mentioning

confidence: 99%

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

et al. 2020

View full text Add to dashboard Cite

Energy storage materials are finding increasing applications in our daily lives, for devices such as mobile phones and electric vehicles. Current commercial batteries use flammable liquid electrolytes, which are unsafe, toxic, and environmentally unfriendly with low chemical stability. Recently, solid electrolytes have been extensively studied as alternative electrolytes to address these shortcomings. Herein, we report the early history, synthesis and characterization, mechanical properties, and Li+ ion transport mechanisms of inorganic sulfide and oxide electrolytes. Furthermore, we highlight the importance of the fabrication technology and experimental conditions, such as the effects of pressure and operating parameters, on the electrochemical performance of all-solid-state Li batteries. In particular, we emphasize promising electrolyte systems based on sulfides and argyrodites, such as LiPS5Cl and β-Li3PS4, oxide electrolytes, bare and doped Li7La3Zr2O12 garnet, NASICON-type structures, and perovskite electrolyte materials. Moreover, we discuss the present and future challenges that all-solid-state batteries face for large-scale industrial applications.

show abstract

“…Different functional approximations exhibit different descriptions of the bulk properties, the chemical bonding, etc. 57,58 In Table 4 of SI we also calculated the relaxed lattice parameters with different functional approximation schemes used in DFT (LDA, 59 PBEsol, 60 PBE with vdw correction 61 and PBE0 62,63 ). These results suggest that PBEsol and PBE with vdw correction offer a better description of the lattice the volume.…”

mentioning

confidence: 99%

Deep Potential generation scheme and simulation protocol for the Li10GeP2S12-type superionic conductors

Huang,

Zhang,

Wang

et al. 2020

Preprint

View full text Add to dashboard Cite

It has been a challenge to accurately simulate Li-ion diffusion processes in battery materials at room temperature using ab initio molecular dynamics (AIMD) due to its high computational cost. This situation has changed drastically in recent years due to the advances in machine learning-based interatomic potentials. Here we implement the Deep Potential Generator scheme to automatically generate interatomic potentials

show abstract

Insights into structural stability and Li superionic conductivity of Li10GeP2S12 from first-principles calculations

Cited by 39 publications

References 22 publications

Origin of Fast Ion Conduction in Li₁₀GeP₂S₁₂, a Superionic Conductor

Origin of Fast Ion Conduction in Li₁₀GeP₂S₁₂, a Superionic Conductor

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

Deep Potential generation scheme and simulation protocol for the Li10GeP2S12-type superionic conductors

Contact Info

Product

Resources

About

Insights into structural stability and Li superionic conductivity of Li10GeP2S12 from first-principles calculations

Cited by 39 publications

References 22 publications

Origin of Fast Ion Conduction in Li10GeP2S12, a Superionic Conductor

Origin of Fast Ion Conduction in Li10GeP2S12, a Superionic Conductor

Sulfide and Oxide Inorganic Solid Electrolytes for All-Solid-State Li Batteries: A Review

Deep Potential generation scheme and simulation protocol for the Li10GeP2S12-type superionic conductors

Contact Info

Product

Resources

About

Origin of Fast Ion Conduction in Li₁₀GeP₂S₁₂, a Superionic Conductor

Origin of Fast Ion Conduction in Li₁₀GeP₂S₁₂, a Superionic Conductor