Atomistic analysis of Li migration in Li1+AlTi2−(PO4)3 (LATP) solid electrolytes

Pfalzgraf, Daniel; Mutter, Daniel; Urban, Daniel F.

doi:10.1016/j.ssi.2020.115521

Cited by 28 publications

(15 citation statements)

References 29 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…tackles exactly these two effects of chemical and geometrical changes in LATP on the Li migration. [ 71 ]…”

Section: Resultsmentioning

confidence: 99%

“…[34][35][36] A recent study by Pfalzgraf et al tackles exactly these two effects of chemical and geometrical changes in LATP on the Li migration. [71] By a model decomposition of macroscopic electrochemical impedance spectroscopy (EIS) data into bulk and interface contributions, Mertens et al had concluded on an orders of magnitude lower interfacial conductivity. [52] The present MD data suggests this lower conductivity to rather arise from limited contact areas or residual secondary phases of extremely ) after computational sintering varied between 40% and 48% of the total simulation cell width total L z .…”

Section: Diffusion Simulations and Ion Conductivitymentioning

confidence: 99%

See 1 more Smart Citation

Nano‐Scale Complexions Facilitate Li Dendrite‐Free Operation in LATP Solid‐State Electrolyte

Stegmaier

Schierholz

Povstugar

et al. 2021

Advanced Energy Materials

View full text Add to dashboard Cite

Over the last two decades, several classes of highly ion-conductive SSEs have been developed which reach or surpass current liquid-state electrolyte conductivity. [5,6] Yet, no ASSB paying in on the above promises has been developed to date. This is mainly due to mechanochemical, chemical, and electrochemical stability issues and interfacial processes that have severely compromised any proposed cell's lifetime. [7][8][9][10][11] While many SSE material inherent (mechano-)chemical processing issues seem amenable to modern engineering approaches, [12][13][14][15][16][17][18][19] the situation is less bright regarding the control of interfacial chemical and electrochemical stability (especially when featuring a LMA), as well as ionic and electronic transport quantities across these interfaces. A hitherto missing deep understanding of the structural, chemical, and physical properties of the buried solid-solid interfaces inside ASSBs at the atomic level is required to overcome these performance limiting interfacial issues.The most studied interfacial properties so far are contact stability and dendrite nucleation and growth. [20][21][22] Both issues are accentuated for LMA/SSE interfaces. In a first approximation, interfacial stability can be traced back to the Dendrite formation and growth remains a major obstacle toward highperformance all solid-state batteries using Li metal anodes. The ceramic Li (1+x) Al (x) Ti (2−x) (PO 4 ) 3 (LATP) solid-state electrolyte shows a higher than expected stability against electrochemical decomposition despite a bulk electronic conductivity that exceeds a recently postulated threshold for dendrite-free operation. Here, transmission electron microscopy, atom probe tomography, and first-principles based simulations are combined to establish atomistic structural models of glass-amorphous LATP grain boundaries. These models reveal a nanometer-thin complexion layer that encapsulates the crystalline grains. The distinct composition of this complexion constitutes a sizable electronic impedance. Rather than fulfilling macroscopic bulk measures of ionic and electronic conduction, LATP might thus gain the capability to suppress dendrite nucleation by sufficient local separation of charge carriers at the nanoscale.

show abstract

“…tackles exactly these two effects of chemical and geometrical changes in LATP on the Li migration. [ 71 ]…”

Section: Resultsmentioning

confidence: 99%

Section: Diffusion Simulations and Ion Conductivitymentioning

confidence: 99%

Nano‐Scale Complexions Facilitate Li Dendrite‐Free Operation in LATP Solid‐State Electrolyte

Stegmaier

Schierholz

Povstugar

et al. 2021

Advanced Energy Materials

View full text Add to dashboard Cite

show abstract

“…analyzed the effect of LATP crystal structure on Li ion migration properties and concluded that the M2 transition state is stabilized due to the increased Al/Ti occupying the octahedral position near the M3 position, which leads to a lower migration potential barrier. [ 96 ] As seen in Figure 3e, He et al. demonstrated the simultaneous occupation of the M1 and M2 sites by Li + , and the strong interaction forces between them can effectively lower the diffusion potential barrier.…”

Section: Microstructure and Conduction Mechanisms Of Latpmentioning

confidence: 99%

Recent Advances in Conduction Mechanisms, Synthesis Methods, and Improvement Strategies for Li₁₊_xAl_xTi₂₋_x(PO₄)₃ Solid Electrolyte for All‐Solid‐State Lithium Batteries

Zhou

et al. 2022

Advanced Energy Materials

View full text Add to dashboard Cite

With the increasing use of Li batteries for storage, their safety issues and energy densities are attracting considerable attention. Recently, replacing liquid organic electrolytes with solid‐state electrolytes (SSE) has been hailed as the key to developing safe and high‐energy‐density Li batteries. In particular, Li1+xAlxTi2−x(PO4)3 (LATP) has been identified as a very attractive SSE for Li batteries due to its excellent electrochemical stability, low production costs, and good chemical compatibility. However, interfacial reactions with electrodes and poor thermal stability at high temperatures severely restrict the practical use of LATP in solid‐state batteries (SSB). Herein, a systematic review of recent advances in LATP for SSBs is provided. This review starts with a brief introduction to the development history of LATP and then summarizes its structure, ion transport mechanism, and synthesis methods. Challenges (e.g., intrinsic brittleness, interfacial resistance, and compatibility) and corresponding solutions (ionic substitution, additives, protective layers, composite electrolytes, etc.) that are critical for practical applications are then discussed. Last, an outlook on the future research direction of LATP‐based SSB is provided.

show abstract

“…Although a large number of SSE materials have been reported, the candidate materials are very limited for solid-state devices. [9][10][11][12] Such as, Li 1+x Al x Ti 2-x (PO 4 ) 3 (LATP), [13][14][15] Li 10 GeP 2 S 12 (LGPS), [16][17][18] and Li x La 2/3-x TiO 3 (LLTO) [19,20] have a high ionic conductivity (10 -3 S cm -1 ) but are not stable against Li metal. LiPON [21][22][23][24] as a chemically stable material for Li exhibits a low ionic conductivity (10 -6 S cm -1 ).…”

Section: Introductionmentioning

confidence: 99%

Garnet Li7La3Zr2O12 Solid-State Electrolyte: Environmental Corrosion, Countermeasures and Applications

Wu¹,

Zhong²,

Zhang³

et al. 2021

ES Energy Environ.

View full text Add to dashboard Cite

Garnet-based Li 7 La 3 Zr 2 O 12 (LLZO), as a popular solid-state electrolyte, is easily corroded by wet air, leading to failure of mechanical strength, Li-ion conductivity and wettability. In this work, corrosion behaviors of garnet electrolyte in air (carbon dioxide, water vapor, CO 2 +H 2 O mixed air, actual moist air) and solution (distilled water, NaCl solution, natural seawater) are investigated, and it is determined that the electrolyte has the worst corrosion resistance to water. Prohibition of direct contact between vapor/liquid water and garnet is the basic design standard. We report a straightforward physical deposition methodology to achieve the growth of poly (vinylidene fluoride) (PVDF) nano-hydrophobic layer on garnet. Grain (R g ) and grain boundary (R gb ) resistances of the electrolyte with PVDF coating are increased by only 14% and 170% at room temperature for 50 hours during a relative humidity of 80%, respectively, which are significantly lower than 930% and 2240% that of the unmodified sample. The modified electrolyte presents the original morphology even after immersed in solution at 353 K for 15 days. Excellent chemical corrosion resistance makes as-prepared garnet have great potential applications in all-solid-state, air-based, and water-based batteries.

show abstract

Atomistic analysis of Li migration in Li1+AlTi2−(PO4)3 (LATP) solid electrolytes

Cited by 28 publications

References 29 publications

Nano‐Scale Complexions Facilitate Li Dendrite‐Free Operation in LATP Solid‐State Electrolyte

Nano‐Scale Complexions Facilitate Li Dendrite‐Free Operation in LATP Solid‐State Electrolyte

Recent Advances in Conduction Mechanisms, Synthesis Methods, and Improvement Strategies for Li₁₊_xAl_xTi₂₋_x(PO₄)₃ Solid Electrolyte for All‐Solid‐State Lithium Batteries

Garnet Li7La3Zr2O12 Solid-State Electrolyte: Environmental Corrosion, Countermeasures and Applications

Contact Info

Product

Resources

About

Atomistic analysis of Li migration in Li1+AlTi2−(PO4)3 (LATP) solid electrolytes

Cited by 28 publications

References 29 publications

Nano‐Scale Complexions Facilitate Li Dendrite‐Free Operation in LATP Solid‐State Electrolyte

Nano‐Scale Complexions Facilitate Li Dendrite‐Free Operation in LATP Solid‐State Electrolyte

Recent Advances in Conduction Mechanisms, Synthesis Methods, and Improvement Strategies for Li1+xAlxTi2−x(PO4)3 Solid Electrolyte for All‐Solid‐State Lithium Batteries

Garnet Li7La3Zr2O12 Solid-State Electrolyte: Environmental Corrosion, Countermeasures and Applications

Contact Info

Product

Resources

About

Recent Advances in Conduction Mechanisms, Synthesis Methods, and Improvement Strategies for Li₁₊_xAl_xTi₂₋_x(PO₄)₃ Solid Electrolyte for All‐Solid‐State Lithium Batteries