The growth mechanism of lithium dendrites and its coupling to mechanical stress

Becherer, Julian; Kramer, Dominik; Mönig, Reiner

doi:10.1039/d1ta10920k

Cited by 14 publications

(16 citation statements)

References 58 publications

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“…This result can be verified indirectly by the experimental results of Rafiz et al 41 who demonstrated that high tortuosity of the separator is effective in preventing dendrite propagation. Kink formation during electrodeposition was reported by Becherer et al 59 using scanning electron microscopy images. When γ = 1 (the pores are not shielded), there are multiple dendrite growth points on the surface of the Li metal; however, owing to the existence of the SM, the transmission path of Li ions is changed significantly, and only the dendrite growth points corresponding to vertically unobstructed pores will eventually grow into dendrites.…”

Section: Influence Of the Degree Of Staggered Overlapmentioning

confidence: 75%

“…This result can be verified indirectly by the experimental results of Rafiz et al who demonstrated that high tortuosity of the separator is effective in preventing dendrite propagation. Kink formation during electrodeposition was reported by Becherer et al . using scanning electron microscopy images.…”

Section: Resultsmentioning

confidence: 99%

“…Newly formed kinks appear either next to another kink or between two kinks (Figure a). The formation of kinks may be due to the regular arrays of dislocations that minimize the energy …”

Section: Resultsmentioning

confidence: 99%

“…The formation of kinks may be due to the regular arrays of dislocations that minimize the energy. 59 Figure 3b shows the distribution of hydrostatic pressure, which indicates the volume change of cells. A negative value represents a tensile state, and a positive value indicates a compressive state.…”

Section: Influence Of the Degree Of Staggered Overlapmentioning

confidence: 99%

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Elucidating the Role of Rational Separator Microstructures in Guiding Dendrite Growth and Reviving Dead Li

Gao

Huang

Guo

2022

ACS Appl. Mater. Interfaces

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Li metal has attracted considerable attention as the preferred anode material for high-energy batteries. However, Li dendrites have limited the development of Li-metal batteries. Herein, the effects of tuning the porous separator microstructure (SM) for guiding Li dendrite growth and reviving dead Li are revealed using a mechano-electrochemical phase-field model. A strategy of guiding, instead of suppression, was applied to avoid disordered Li dendrite growth. By analyzing the effects of the number of layers, thickness, degree of staggered overlap in the separator, interlayer spacing, and porosity of SM on Li dendrite behavior, we discovered that applying a rationally designed SM can finely guide the Li nucleation and growth direction toward dense deposition. The revival of dead Li was also observed via an in situ experiment on Li dendrites. The reactivation of dead Li after it recontacts Li metal was verified. These findings not only provide fundamental information for the tuning of the SM but can also help better understand the dendrite growth of other alkali metal-ion batteries.

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Section: Influence Of the Degree Of Staggered Overlapmentioning

confidence: 75%

Section: Resultsmentioning

confidence: 99%

“…Newly formed kinks appear either next to another kink or between two kinks (Figure a). The formation of kinks may be due to the regular arrays of dislocations that minimize the energy …”

Section: Resultsmentioning

confidence: 99%

Section: Influence Of the Degree Of Staggered Overlapmentioning

confidence: 99%

See 2 more Smart Citations

Elucidating the Role of Rational Separator Microstructures in Guiding Dendrite Growth and Reviving Dead Li

Gao

Huang

Guo

2022

ACS Appl. Mater. Interfaces

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“…Both effects lead to capacity loss and are enhanced with increasingly irregular, nonplanar, and high-surface-area structures of the lithium anode. Experiments have found that the nonplanar structure arises from whiskers, growing with no apparent growth direction during charging. − Lithium whiskers, often with small diameters, entangle each other to form mossy lithium . The growth process is not limited by electrolyte transport at battery-typical current densities. − During discharging, portions of lithium remain isolated in the SEI shell. ,, This isolated lithium can accumulate at the electrode, increasing the cell resistance because the ion path becomes tortuous − or floats in the electrolyte and possibly reacts at high voltage and elevated temperatures .…”

mentioning

confidence: 99%

Origin of Heterogeneous Stripping of Lithium in Liquid Electrolytes

Werres

Jia

et al. 2023

ACS Nano

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Lithium metal batteries suffer from low cycle life. During discharge, parts of the lithium are not stripped reversibly and remain isolated from the current collector. This isolated lithium is trapped in the insulating remaining solid-electrolyte interphase (SEI) shell and contributes to the capacity loss. However, a fundamental understanding of why isolated lithium forms and how it can be mitigated is lacking. In this article, we perform a combined theoretical and experimental study to understand isolated lithium formation during stripping. We derive a thermodynamic consistent model of lithium dissolution and find that the interaction between lithium and SEI leads to locally preferred stripping and isolated lithium formation. Based on a cryogenic transmission electron microscopy (cryo TEM) setup, we reveal that these local effects are particularly pronounced at kinks of lithium whiskers. We find that lithium stripping can be heterogeneous both on a nanoscale and on a larger scale. Cryo TEM observations confirm our theoretical prediction that isolated lithium occurs less at higher stripping current densities. The origin of isolated lithium lies in local effects, such as heterogeneous SEI, stress fields, or the geometric shape of the deposits. We conclude that in order to mitigate isolated lithium, a uniform lithium morphology during plating and a homogeneous SEI are indispensable.

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In Situ Engineering of Inorganic‐Rich Solid Electrolyte Interphases via Anion Choice Enables Stable, Lithium Anodes

Weeks,

Burrow,

Diao

et al. 2023

Advanced Materials

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The discovery of liquid battery electrolytes that facilitate the formation of stable solid electrolyte interphases (SEIs) to mitigate dendrite formation is imperative to enable lithium anodes in next‐generation energy‐dense batteries. Compared to traditional electrolyte solvents, tetrahydrofuran (THF)‐based electrolyte systems have demonstrated great success in enabling high‐stability lithium anodes by encouraging the decomposition of anions (instead of organic solvent) and thus generating inorganic‐rich SEIs. Herein, by employing a variety of different lithium salts (i.e., LiPF6, LiTFSI, LiFSI, and LiDFOB), we demonstrate that electrolyte anions modulate the inorganic composition and resulting properties of the SEI. Through novel analytical ToF‐SIMS methods, such as hierarchical clustering of depth profiles and compositional analysis using integrated yields, we examine the chemical composition and morphology of the SEIs generated from each electrolyte system. Notably, the LiDFOB electrolyte provides an exceptionally stable system to enable lithium anodes, delivering > 1500 cycles at a current density of 0.5 mAh g−1 and a capacity of 0.5 mAh g−1 in symmetrical cells. Furthermore, Li//LFP cells using this electrolyte demonstrate high‐rate, reversible lithium storage, supplying 139 mAh g(LFP)−1 at C/2 (∼ 0.991 mAh cm−2, @ 0.61 mA cm−2) with 87.5% capacity retention over 300 cycles (average Coulombic efficiency >99.86%).This article is protected by copyright. All rights reserved

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The growth mechanism of lithium dendrites and its coupling to mechanical stress

Abstract: Operando high-resolution light microscopy with extended depth of field is used to observe large regions of an electrode during electrodeposition of lithium. The analysis of the morphology of the evolving...

Cited by 14 publications

References 58 publications

Elucidating the Role of Rational Separator Microstructures in Guiding Dendrite Growth and Reviving Dead Li

Elucidating the Role of Rational Separator Microstructures in Guiding Dendrite Growth and Reviving Dead Li

Origin of Heterogeneous Stripping of Lithium in Liquid Electrolytes

In Situ Engineering of Inorganic‐Rich Solid Electrolyte Interphases via Anion Choice Enables Stable, Lithium Anodes

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