In-situ, non-destructive acoustic characterization of solid state electrolyte cells

Schmidt, Robert D.; Sakamoto, Jeffrey

doi:10.1016/j.jpowsour.2016.05.062

Cited by 58 publications

(39 citation statements)

References 44 publications

(84 reference statements)

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“…a,b,d) Secondary electron images of the fracture surface. Factors that could be responsible for this behavior include localized thermodynamic and kinetic effects, [33,34] stress distribution in the solid electrolyte, and subcritical mechanical damage ahead of the filament tip. Samples in (a)-(c) were exposed to air for <1 min while the sample in (d) was transported in a vacuum operated transfer box.…”

Section: Resultsmentioning

confidence: 99%

“…[23][24][25][26][27] Several attempts to suppress the shorting via solid electrolyte composition alterations and electrode/solid electrolyte interfacial modifications have been made, [24,[28][29][30][31] but with limited success. As pointed out in two recent reports, [33,34] similar short circuit events were investigated in Na-ion conducting solid electrolytes in liquid Na batteries in the 1970-1980s. [32] The reasons for this difference in behavior between bulk and thin film batteries are not understood.…”

Section: Introductionmentioning

confidence: 86%

See 1 more Smart Citation

Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

Porz

Swamy

Sheldon

et al. 2017

Advanced Energy Materials

844

973

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vast improvements in energy density may be achieved with lithium metal anodes owing to their high gravimetric capacity (3869 mA h g −1 ) and low density (0.534 g cm −3 ). However, adoption of rechargeable lithium metal batteries has been unsuccessful thus far due to safety concerns associated with short circuits that occur when Li dendrites grow through the liquid electrolyte during the charging process. [4][5][6] Although several approaches have reduced dendrite formation, [7][8][9][10] to date the phenomenon has not been avoided under all relevant conditions. Nonflammable inorganic solid electrolytes, paired with Li metal anodes, could result in high energy density yet safe rechargeable lithium batteries. [11][12][13][14][15] As reviewed by Takada, [12] inorganic solid electrolytes have now been widely studied, [16][17][18][19][20] but are not yet commercialized. Monroe and Newman have suggested that dendrite growth during the plating process may be suppressed if the liquid electrolyte is replaced with a Li-ion conducting solid electrolyte of a sufficiently high shear modulus. [21,22] According to this criterion, numerous inorganic solid electrolytes should be able to suppress dendrite formation. However, multiple research groups have recently reported cases where ceramic solid electrolytes paired with a Li metal anode experience a short circuit Li deposition is observed and measured on a solid electrolyte in the vicinity of a metallic current collector. Four types of ion-conducting, inorganic solid electrolytes are tested: Amorphous 70/30 mol% Li 2 S-P 2 S 5 , polycrystalline β-Li 3 PS 4 , and polycrystalline and single-crystalline Li 6 La 3 ZrTaO 12 garnet. The nature of lithium plating depends on the proximity of the current collector to defects such as surface cracks and on the current density. Lithium plating penetrates/infiltrates at defects, but only above a critical current density. Eventually, infiltration results in a short circuit between the current collector and the Li-source (anode). These results do not depend on the electrolytes shear modulus and are thus not consistent with the Monroe-Newman model for "dendrites." The observations suggest that Li-plating in pre-existing flaws produces crack-tip stresses which drive crack propagation, and an electrochemomechanical model of plating-induced Li infiltration is proposed. Lithium short-circuits through solid electrolytes occurs through a fundamentally different process than through liquid electrolytes. The onset of Li infiltration depends on solid-state electrolyte surface morphology, in particular the defect size and density.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 86%

Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

Porz

Swamy

Sheldon

et al. 2017

Advanced Energy Materials

844

973

View full text Add to dashboard Cite

show abstract

“…This scenario was further validated by continuum mechanics simulations, as detailed in Figure S1 (Supporting Information), which shows that the lithium‐ion current density is locally concentrated at asperity flaws. This inhomogeneous lithium deposition acts as a source of mechanical pressure that facilitates the formation of voids and contact loss, leading to cell failure 22,24,39. Since morphological defects on the LLZO surface are inevitable to some extent during manufacturing, an appropriate approach that mitigates this problem needs to be devised.…”

Section: Resultsmentioning

confidence: 99%

The Role of Interlayer Chemistry in Li‐Metal Growth through a Garnet‐Type Solid Electrolyte

Kim

Jung

Kim

et al. 2020

Advanced Energy Materials

131

130

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Securing the chemical and physical stabilities of electrode/solid‐electrolyte interfaces is crucial for the use of solid electrolytes in all‐solid‐state batteries. Directly probing these interfaces during electrochemical reactions would significantly enrich the mechanistic understanding and inspire potential solutions for their regulation. Herein, the electrochemistry of the lithium/Li7La3Zr2O12‐electrolyte interface is elucidated by probing lithium deposition through the electrolyte in an anode‐free solid‐state battery in real time. Lithium plating is strongly affected by the geometry of the garnet‐type Li7La3Zr2O12 (LLZO) surface, where nonuniform/filamentary growth is triggered particularly at morphological defects. More importantly, lithium‐growth behavior significantly changes when the LLZO surface is modified with an artificial interlayer to produce regulated lithium depositions. It is shown that lithium‐growth kinetics critically depend on the nature of the interlayer species, leading to distinct lithium‐deposition morphologies. Subsequently, the dynamic role of the interlayer in battery operation is discussed as a buffer and seed layer for lithium redistribution and precipitation, respectively, in tailoring lithium deposition. These findings broaden the understanding of the electrochemical lithium‐plating process at the solid‐electrolyte/lithium interface, highlight the importance of exploring various interlayers as a new avenue for regulating the lithium‐metal anode, and also offer insight into the nature of lithium growth in anode‐free solid‐state batteries.

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“…However, for typical SSEs, an alternative failure mode is the propagation of pre-existing interfacial defects, namely Griffith flaws. 30 During electrodeposition through the solid electrolyte, such interfacial flaws are the first to fill with metal, schematically shown in Figure 1. As additional metal arrives at the tip of the flaw where electric field is largest, a competition arises between propagation of the metal filament into the solid electrolyte and extrusion of the metal backwards, to accommodate volume increase.…”

Section: Solid Electrolyte Mechanical Considerationsmentioning

confidence: 99%

“…Schmidt and Sakamoto report in-situ acoustic experiments related to this mechanism finding that a reduction in SSE stiffness accompanies Li penetration, consistent with crack propagation. 30 According to this theory, the ability of all-solid-state batteries to cycle without Li penetration related failures is predicated on defect-free layers. Correspondingly, the growing number of observations of metal penetration through high modulus SSEs, observed in cycling of Li symmetric cells, 9,[33][34][35] can likely be explained by preexisting interfacial defects.…”

Section: Solid Electrolyte Mechanical Considerationsmentioning

confidence: 99%

Review—Practical Challenges Hindering the Development of Solid State Li Ion Batteries

Kerman

Luntz

Viswanathan

et al. 2017

J. Electrochem. Soc.

562

471

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Solid state electrolyte systems boasting Li + conductivity of >10 mS cm −1 at room temperature have opened the potential for developing a solid state battery with power and energy densities that are competitive with conventional liquid electrolyte systems. The primary focus of this review is twofold. First, differences in Li penetration resistance in solid state systems are discussed, and kinetic limitations of the solid state interface are highlighted. Second, technological challenges associated with processing such systems in relevant form factors are elucidated, and architectures needed for cell level devices in the context of product development are reviewed. Specific research vectors that provide high value to advancing solid state batteries are outlined and discussed. Solid state battery systems are of great interest because of potential benefits in gravimetric and volumetric energy density, operable temperature range, and safety in comparison to traditional liquid electrolyte based systems. However, unresolved fundamental issues remain in the quest to fully understand the behavior of all-solid batteries, especially in the area of electrochemical interfaces.1 There are also a number of significant engineering challenges that require methodical effort to enable a tangible product. Some transitions from academic laboratories to entrepreneurial efforts attempting to overcome these challenges remain unsuccessful in efforts to bring a product to the market.2,3 Vital parameters that require robust understanding from a product development standpoint are material cost, cell lifetime and shelf life, cell energy density on a volumetric and gravimetric basis, operable capabilities for given temperature conditions, and safety. The advantage of energy density remains to be realized in solid state electrolytes (SSEs) since most studies to date utilize thick SSEs or cathodes with low active loading compared to liquid counterparts. 4,5 Furthermore, the desire to use SSEs in conjunction with Li metal anodes requires understanding and managing the morphology of Li metal plating, which can impact volumetric energy density. Operation at both higher and lower temperature compared to conventional technologies is a significant potential advantage of SSE systems. However, reports of solid state cells achieving parity with traditional systems at room temperature or any other temperature do not currently exist. The safety, specifically decreased flammability, of SSE systems is another potential advantage but requires ongoing validation and study.6 Unlike current liquid electrolyte systems, 7 the manufacturability and material component costs of SSEs have not been well characterized, and thus the value of these features will need to be weighed accordingly with any added cost. Operating lifetime of SSEs capturing intrinsic materials parameters such as voltage stability, 8 as well as catastrophic failure modes such as shorting, 9 have been briefly investigated, but in the absence of high energy density electrode formulations and appli...

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In-situ, non-destructive acoustic characterization of solid state electrolyte cells

Cited by 58 publications

References 44 publications

Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

Mechanism of Lithium Metal Penetration through Inorganic Solid Electrolytes

The Role of Interlayer Chemistry in Li‐Metal Growth through a Garnet‐Type Solid Electrolyte

Review—Practical Challenges Hindering the Development of Solid State Li Ion Batteries

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