Thin laminar inorganic solid electrolyte with high ionic conductance towards high-performance all-solid-state lithium battery

Guo, Shiyuan; Kou, Weijie; Wu, Wenjia; Lv, Ruixin; Yang, Zhihao; Wang, Jingtao

doi:10.1016/j.cej.2021.131948

Cited by 36 publications

(17 citation statements)

References 58 publications

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“…This presents two important factors for dendrite formation and propagation: (1) the heterogeneity shows regions of pure polymer amid the LLZO mixture, and (2) wherever there is LLZO present, its effective modulus is lower than pure LLZO, either due to inherently lower modulus at the nanoscale or due to being covered by a thin layer of PEO-LiTFSI. These modulus ranges lower than the Young’s modulus of lithium metal (5–11 GPa) have been observed previously in LLZO nanosheets and composite electrolytes with nanoindentation. , …”

Section: Results and Discussionmentioning

confidence: 45%

“…These modulus ranges lower than the Young's modulus of lithium metal (5−11 GPa) have been observed previously in LLZO nanosheets and composite electrolytes with nanoindentation. 55,56 Figure 5b compares these numbers with those of LLZO and lithium metal reported in the literature at room temperature. 57 Also shown is the shear modulus, estimated from the relationship G = E/(2 × (1 + ν)), where G is the shear modulus, E is the Young's modulus, and ν is the Poisson's ratio, which is around 0.25 for both LLZO and solid polymer electrolytes.…”

Section: Effect Of Fiber Loading On Ce and Ccd Our Resultsmentioning

confidence: 74%

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Understanding the Influence of Li₇La₃Zr₂O₁₂ Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes

Counihan,

Powers,

Barai

et al. 2023

ACS Appl. Mater. Interfaces

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Composite polymer electrolytes (CPEs) are attractive materials for solid-state lithium metal batteries, owing to their high ionic conductivity from ceramic ionic conductors and flexibility from polymer components. As with all lithium metal batteries, however, CPEs face the challenge of dendrite formation and propagation. Not only does this lower the critical current density (CCD) before cell shorting, but the uncontrolled growth of lithium deposits may limit Coulombic efficiency (CE) by creating dead lithium. Here, we present a fundamental study on how the ceramic components of CPEs influence these characteristics. CPE membranes based on poly(ethylene oxide) and lithium bis(trifluoromethanesulfonyl)imide (PEO-LiTFSI) with Li7La3Zr2O12 (LLZO) nanofibers were fabricated with industrially relevant roll-to-roll manufacturing techniques. Galvanostatic cycling with lithium symmetric cells shows that the CCD can be tripled by including 50 wt % LLZO, but half-cell cycling reveals that this comes at the cost of CE. Varying the LLZO loading shows that even a small amount of LLZO drastically lowers the CE, from 88% at 0 wt % LLZO to 77% at just 2 wt % LLZO. Mesoscale modeling reveals that the increase in CCD cannot be explained by an increase in the macroscopic or microscopic stiffness of the electrolyte; only the microstructure of the LLZO nanofibers in the PEO-LiTFSI matrix slows dendrite growth by presenting physical barriers that the dendrites must push or grow around. This tortuous lithium growth mechanism around the LLZO is corroborated with mass spectrometry imaging. This work highlights important elements to consider in the design of CPEs for high-efficiency lithium metal batteries.

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Section: Results and Discussionmentioning

confidence: 45%

Section: Effect Of Fiber Loading On Ce and Ccd Our Resultsmentioning

confidence: 74%

Understanding the Influence of Li₇La₃Zr₂O₁₂ Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes

Counihan,

Powers,

Barai

et al. 2023

ACS Appl. Mater. Interfaces

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“…prepared a freestanding LLZO laminar membrane by vacuum filtrating LLZO nanosheets followed by PEO/LiTFSI infiltration (Figure 6D,E). 81 Due to the laminar framework of LLZO, LLZO‐PEO electrolyte shows a compressive strength of 3.2 GPa, which is 10 times higher than the CPE composed of randomly orientated LLZO nanosheets (Figure 6F). The improved mechanical properties show advantages in suppressing Li dendrite penetration in Li/Li symmetric cell testing.…”

Section: Horizontally Ordered Ssesmentioning

confidence: 96%

“…(D) Schematic illustration of the production of Li 7 La 3 Zr 2 O 12 (LLZO)‐PEO electrolyte, (E) its cross‐section SEM image, and (F) load‐displacement curves. Reproduced with permission 81 . Copyright 2022, Elsevier…”

Section: Horizontally Ordered Ssesmentioning

confidence: 99%

Order‐structured solid‐state electrolytes

Rao

Wang

et al. 2022

SusMat

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Solid-state electrolytes (SSEs) are recognized as attractive candidates to realize safe and high-energy-density lithium metal batteries (LMBs). However, the practical application of SSEs still faces challenges such as insufficient roomtemperature ionic conductivity, unsatisfactory mechanical properties, and large internal resistance. Extensive research efforts have been made to explore new electrochemistry and technologies to address those challenges. Among them, the construction of order-structured SSEs has emerged as a promising strategy.The anisotropic behavior induced by the orientation offers SSEs with desired properties targeting specific functions, and therefore the rational design of the order-structured SSE provides an alternative solution to achieve an ideal SSE. This review discusses the structure-property correlation of SSEs, and then summarizes the design strategies to construct order-structured SSEs. Finally, the current challenges and possible future research directions for order-structured SSEs for scalable high-energy-density LMBs are presented.

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“…(c) Long cycling of the cells tests at 60 °C. (d) Active mass loading and cycle number of the garnet-based SSLMBs in our work compared with reported literatures using various interface engineering strategies. − (e, f) Variation of Li-ion concentration on the surface of electrode particles through finite element analysis in (e) Model 1 with low σ and and (f) Model 2 with high σ and .…”

mentioning

confidence: 94%

Solvent-Free and Long-Cycling Garnet-Based Lithium-Metal Batteries

Zhai

Zhang

et al. 2023

ACS Energy Lett.

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Solid-state batteries using ceramic solid electrolytes promise to deliver enhanced energy density and intrinsic safety. However, the challenge of integrating solid electrolytes with electrode materials limits the electrochemical performance. Herein, we report a solvent-free ceramic-based lithium-metal battery with good cycling stability at a wide temperature range from 45 to 100 °C, enabled by an inorganic ternary salt of low eutectic point. By using a garnet electrolyte with molten salts at the electrolyte|cathode interface, the Li||LiFePO4 cells perform a long cycling with capacity retention of 81.4% after 1000 cycles at 1 C. High-voltage LiFe0.4Mn0.6PO4 cathodes also deliver good electrochemical performance. Specifically, commercial electrode pieces with high area capacities can be adopted directly in the quasi-solid-state lithium-metal batteries. These stable performances are ascribable to the low melting point, high ionic conductivity and good thermal/electrochemical stability of the ternary salt system. Our findings provide an effective method on fabrication of solid-state batteries for practical applications.

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Thin laminar inorganic solid electrolyte with high ionic conductance towards high-performance all-solid-state lithium battery

Cited by 36 publications

References 58 publications

Understanding the Influence of Li₇La₃Zr₂O₁₂ Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes

Understanding the Influence of Li₇La₃Zr₂O₁₂ Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes

Order‐structured solid‐state electrolytes

Solvent-Free and Long-Cycling Garnet-Based Lithium-Metal Batteries

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Thin laminar inorganic solid electrolyte with high ionic conductance towards high-performance all-solid-state lithium battery

Cited by 36 publications

References 58 publications

Understanding the Influence of Li7La3Zr2O12 Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes

Understanding the Influence of Li7La3Zr2O12 Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes

Order‐structured solid‐state electrolytes

Solvent-Free and Long-Cycling Garnet-Based Lithium-Metal Batteries

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Product

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Understanding the Influence of Li₇La₃Zr₂O₁₂ Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes

Understanding the Influence of Li₇La₃Zr₂O₁₂ Nanofibers on Critical Current Density and Coulombic Efficiency in Composite Polymer Electrolytes