Rate-dependent deformation of amorphous sulfide glass electrolytes for solid-state batteries

Athanasiou, Christos E.; Liu, Xing; Jin, Mok Yun; Nimon, Eugene; Visco, Steven J.; Lee, Cholho; Park, Myounggu; Yun, Junnyeong; Padture, Nitin P.; Gao, Huajian; Sheldon, Brian W.

doi:10.1016/j.xcrp.2022.100845

Cited by 15 publications

(19 citation statements)

References 42 publications

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“…The images in Figure demonstrate that the shapes of the original molds are well-preserved on the patterned SE surface, even after final compaction/densification. This demonstrates the benefits of using the LPSC SE in the molding process, which can easily plastically deform into the mold shape because of its relatively low yield strength. ,, …”

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confidence: 86%

“…This demonstrates the benefits of using the LPSC SE in the molding process, which can easily plastically deform into the mold shape because of its relatively low yield strength. 12,16,54 In addition to the mechanical properties of the SE, the material properties and geometric shape of the mold must also be carefully selected to survive the templating process under the applied loads. The mold material must be sufficiently stiff (elastic modulus), strong (yield strength), and tough (fracture toughness) to avoid mechanical failure during the templating process.…”

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confidence: 99%

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Improved Rate Capability in Composite Solid-State Battery Electrodes Using 3-D Architectures

et al. 2023

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The limited rate capability observed at faster charging rates is a critical challenge for composite electrodes in solid-state batteries (SSBs). This becomes further amplified with increasing electrode thickness and higher ratios of active material to solid electrode, which result in tradeoffs between energy and power density. To overcome these trade-offs, it is necessary to understand the factors responsible for poor rate capability by exploring new approaches to boost power density without compromising energy density. Herein, we fabricated 3-D patterned composite graphite (Gr/Li 6 PS 5 Cl) electrodes with low-tortuosity electrolyte channels using a templating approach. Graphite was chosen as a model system to study inhomogeneous lithiation in composite SSB electrode architectures because of the visible color changes that occur as a function of local state-of-charge. At faster cycling rates (1C), the 3-D patterned electrodes enabled considerably higher accessible capacity (38% increase) compared to the unpatterned control electrodes. These enhancements were visualized using operando video microscopy, where 3-D electrode architectures showed improved homogeneity in the local state-of-charge throughout the electrode thickness. The insights presented here will enable new strategies based on 3-D electrode architectures to overcome power/energy trade-offs in SSBs.

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confidence: 99%

Improved Rate Capability in Composite Solid-State Battery Electrodes Using 3-D Architectures

et al. 2023

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“…[12] This behavior is likely due to the lower yield strength of sulfides, especially compared to the hard and brittle nature of oxides such as LLZO. [37,38] The ability of the SSE to locally deform to contact the current collector is an important factor in developing high-performance anode-free SSBs. We note that in contrast to LLZO, LPSC is not thermodynamically stable in contact with lithium, but the interphase layer only grows to be ≈250 nm thick.…”

Section: Resultsmentioning

confidence: 99%

“…This result contrasts with the challenges of interfacing an anode-free current collector with oxides, such as LLZO, which have required hot pressing at temperatures > 900 °C to form a viable interface 12 . This behavior is likely due to the lower yield strength of sulfides, especially compared to the hard and brittle nature of oxides like LLZO 36,37 . The ability of the SSE to locally deform to contact the current collector is thus an important factor in developing high-performance anode-free SSBs.…”

Section: Lithium Deposition Behavior At Anode-free Interfacesmentioning

confidence: 99%

Accelerated Short Circuiting in Anode‐Free Solid‐State Batteries Driven by Local Lithium Depletion

Lewis

Sandoval

Liu

et al. 2023

Advanced Energy Materials

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Anode-free" solid-state batteries (SSBs), which have no active material at the anode and undergo in situ lithium plating during the first charge, can exhibit extremely high energy density (~1500 Wh L -1 ). However, there is a lack of understanding of lithium plating/stripping mechanisms at bare solid-state electrolyte (SSE) interfaces since excess lithium is often used. Here, we demonstrate that commercially relevant quantities of lithium (> 5 mAh cm -2 ) can be reliably plated at relatively high current densities (1 mA cm -2 ) using the sulfide SSE Li6PS5Cl. Investigations of lithium plating/stripping mechanisms, in conjunction with cryo-focused ion beam (FIB) and ex situ synchrotron tomography, reveal that the cycling stability of these cells is intrinsically limited by spatially uneven plating/stripping. Local lithium depletion toward the end of stripping decreases electrochemically active area, which results in high local current densities and void formation, accelerating subsequent filament growth and short circuiting compared to lithium-excess cells.Despite this governing degradation mode, we show that anode-free cells exhibit comparable Coulombic efficiencies to lithium-excess cells before short circuiting, and improved resistance to short-circuiting is achieved by avoiding local lithium depletion through retention of lithium at the interface. These new insights provide a foundation for engineering future high-energy anode-free SSBs.

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“…Moreover, the active material breathing will be transferred to the solid electrolyte that will subsequently need to adapt to the local change. Sulfide solid electrolyte have interesting mechanical properties with a Young moduli around 20 GPa and generally able to manage little volume change, especially true when amorphous solid electrolyte are employed since the stress/strain cannot propagate along grains boundaries. − Additionally, one should pay attention to the pressure used for cycling which is independent from the one applied for the sintering of the solid electrolyte/composite electrode. − Indeed, when the sintering is properly performed in the solid electrolyte and on the composite electrode, there is no need for a strong pressure to be applied on the cell for cycling. However, the story is different when the cell stack is fully assembled and the counter electrode needs to be properly “attached” to the separator, which has a certain surface rugosity.…”

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confidence: 99%

Composite Electrode (LiNi_0.6Mn_0.2Co_0.2O₂) Engineering for Thiophosphate Solid-State Batteries: Morphological Evolution and Electrochemical Properties

Perrenot,

Bayle-Guillemaud,

Villevieille

2023

ACS Energy Lett.

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Solid-state batteries using thiophosphate solid electrolytes are believed to be the next generation solid electrolyte batteries, but they suffer from several issues, including also the engineering of the composite positive electrode. To date, the relationship between the morphology of the composite electrode and its electrochemical performance remains undetermined. By using Focused Ion Beam–Scanning Electron Microscopy (FIB-SEM) tomography, we investigated the engineering of several composite electrodes of polycrystalline NMC 622 (LiNi0.6Mn0.2Co0.2O2) particles and amorphous Li3PS4 solid electrolyte. Based on the morphological analysis of the electronic and ionic networks, it is possible to determine that the electrochemical performance limitation in this cell emerges from the surface contact between the NMC and the LPS as the sintering of the solid electrolyte (SE) is far from optimal. Additionally, similar analyses performed after the first charge show that the fading of the electrochemical is linked to the morphological evolution in the composite positive electrode.

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Rate-dependent deformation of amorphous sulfide glass electrolytes for solid-state batteries

Cited by 15 publications

References 42 publications

Improved Rate Capability in Composite Solid-State Battery Electrodes Using 3-D Architectures

Improved Rate Capability in Composite Solid-State Battery Electrodes Using 3-D Architectures

Accelerated Short Circuiting in Anode‐Free Solid‐State Batteries Driven by Local Lithium Depletion

Composite Electrode (LiNi_0.6Mn_0.2Co_0.2O₂) Engineering for Thiophosphate Solid-State Batteries: Morphological Evolution and Electrochemical Properties

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Rate-dependent deformation of amorphous sulfide glass electrolytes for solid-state batteries

Cited by 15 publications

References 42 publications

Improved Rate Capability in Composite Solid-State Battery Electrodes Using 3-D Architectures

Improved Rate Capability in Composite Solid-State Battery Electrodes Using 3-D Architectures

Accelerated Short Circuiting in Anode‐Free Solid‐State Batteries Driven by Local Lithium Depletion

Composite Electrode (LiNi0.6Mn0.2Co0.2O2) Engineering for Thiophosphate Solid-State Batteries: Morphological Evolution and Electrochemical Properties

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Composite Electrode (LiNi_0.6Mn_0.2Co_0.2O₂) Engineering for Thiophosphate Solid-State Batteries: Morphological Evolution and Electrochemical Properties