Electrodeposition and Mechanical Stability at Lithium-Solid Electrolyte Interface during Plating in Solid-State Batteries

Tu, Qingsong; Barroso-Luque, Luis; Shi, Tan; Ceder, Gerbrand

doi:10.1016/j.xcrp.2020.100106

Cited by 89 publications

(108 citation statements)

References 56 publications

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“…K is obtained by calibrating the resulting stress at the interface to the calculated stress reported in analytical and computational works. [ 26,34,35 ] Full description of this electro‐chemo‐mechanical phase‐field model can be found in Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

“…Moreover, the theoretical studies show the interfacial stress is on the order of a few megapascals. [ 26,34–36 ] Thus, through the calibration, the constants related to the inelastic strain are determined to be K ii = 2.1 × 10 −4 . All simulation parameters are listed in Table S1 (Supporting Information) and more details can be found in Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

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Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Tantratian

Yan

Ellwood

et al. 2021

Advanced Energy Materials

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Lithium dendrite penetration has been widely evidenced in ceramic solid electrolytes (SEs), which are expected to suppress Li dendrite formation due to their ultrahigh elastic modulus. This work aims to reveal the mechanism of Li penetration in polycrystalline SEs through electro‐chemo‐mechanical phase‐field model, using Li7La3Zr2O12 (LLZO) as the model material. The results show the Li penetration patterns are influenced by both mechanical and electronic properties of the microstructures, i.e., grain boundaries (GBs). Li nucleates at the GB junctions on the Li/SE interface and propagates along the GB, at which the interfacial compressive stress is small due to the GB softening. Moreover, the excess trapped electrons at the GB may trigger isolated Li nucleation sites, abruptly increasing the Li penetration depth. High‐throughput simulations yield a phase map of Li penetration patterns under different trapped electrons concentrations and GB/grain elastic modulus mismatch. The map can quantitatively inform whether the mechanical or electronic properties dominate Li penetration morphologies, providing a strategy for the design of improved SE materials.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Tantratian

Yan

Ellwood

et al. 2021

Advanced Energy Materials

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“…predicted mechanical stability for sulfide SEs up to 160 MPa, which means that a stack pressure induced SE fracture that could induce the short circuit can be excluded at <125 MPa. [ 18 ] We believe that the instant mechanical shorting is triggered by the extrusion of metallic lithium through the entire thickness of the SE pellet, as explained below. Figure 1b shows the impedance response of the Li‐cell before (74 MPa) and after (125 MPa) the instant mechanically induced short circuit.…”

Section: Resultsmentioning

confidence: 99%

“…It might be that a stack pressure of 11 MPa is not high enough to fully extrude the lithium through the entire SE pellet (see below), but even a minimal extrusion into the cracks of the SE pellet has a dramatic impact on the electrochemical behavior of the symmetric Li|Li 6 PS 5 Cl|Li cell (Figure S6b, Supporting Information). The extruded lithium becomes the preferential stripping and plating site as the ionic path length is shorter, [ 18 ] as schematically shown in Figure 3d. This results in inhomogeneous stripping and plating, which accelerates the penetration of the metallic lithium through the SE and results in an electrochemically induced short circuit of the Li|Li 6 PS 5 Cl|Li cell only after a few stripping and plating cycles.…”

Section: Resultsmentioning

confidence: 99%

The Stack Pressure Dilemma in Sulfide Electrolyte Based Li Metal Solid‐State Batteries: A Case Study with Li₆PS₅Cl Solid Electrolyte

Hänsel

Kundu

2021

Adv Materials Inter

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Lithium–solid electrolyte (SE) improper contact and morphological instabilities at the interface during Li plating and stripping are two critical problems that may hinder the realization of Li metal solid‐state batteries (SSBs). While the application of a substantial stack pressure during battery operation can potentially overcome these issues, its proper metering is challenging, especially, when Li metal is employed as the anode, as demonstrated here with Li6PS5Cl as the SE. The low yield strength of Li leads to its extrusion through the micropores of a considerably dense (≈92%) SE even under a moderate stack pressure, resulting in mechanically induced short circuit, which is expedited with decreasing SE thickness. This predicament is avoided at low stack pressures, but inhomogeneous Li plating/stripping triggers dendritic failure at higher currents. Besides highlighting the significance of assembly pressure on the Li‐SSB performance, a comprehensive understanding of the too much versus too little stack pressure dilemma is presented here, which can potentially guide the development of strategies to overcome the electrochemomechanical issues at the Li–SE interface.

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“…287,288 The use of a Li metal anode results in additional issues of contact loss during plating/stripping, possible interfacial reactions, and Li propagation through the conductor. 214,215,217,289 Most of these mechanical and chemical interfacial instabilities increase the overpotential, resulting in lower energy density and capacity fade. Finally, practical cells will also require very thin SE separators that are easily processed and handled, and high cathode loading, which are issues that have only been partially addressed so far by the scientific community.…”

Section: Challenges Facing Assbsmentioning

confidence: 99%

Promises and Challenges of Next-Generation “Beyond Li-ion” Batteries for Electric Vehicles and Grid Decarbonization

et al. 2020

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The tremendous improvement in performance and cost of lithium-ion batteries (LIBs) have made them the technology of choice for electrical energy storage. While established battery chemistries and cell architectures for Li-ion batteries achieve good power and energy density, LIBs are unlikely to meet all the performance, cost, and scaling targets required for energy storage, in particular, in large-scale applications such as electrified transportation and grids. The demand to further reduce cost and/or increase energy density, as well as the growing concern related to natural resource needs for Li-ion have accelerated the investigation of so-called "beyond Li-ion" technologies. In this review, we will discuss the recent achievements, challenges, and opportunities of four important "beyond Li-ion" technologies: Na-ion batteries, K-ion batteries, all-solid-state batteries, and multivalent batteries. The fundamental science behind the challenges, and potential solutions toward the goals of a low-cost and/or high-energy-density future, are discussed in detail for each technology. While it is unlikely that any given new technology will fully replace Li-ion in the near future, "beyond Li-ion" technologies should be thought of as opportunities for energy storage to grow into mid/large-scale applications.

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Electrodeposition and Mechanical Stability at Lithium-Solid Electrolyte Interface during Plating in Solid-State Batteries

Cited by 89 publications

References 56 publications

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

The Stack Pressure Dilemma in Sulfide Electrolyte Based Li Metal Solid‐State Batteries: A Case Study with Li₆PS₅Cl Solid Electrolyte

Promises and Challenges of Next-Generation “Beyond Li-ion” Batteries for Electric Vehicles and Grid Decarbonization

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Electrodeposition and Mechanical Stability at Lithium-Solid Electrolyte Interface during Plating in Solid-State Batteries

Cited by 89 publications

References 56 publications

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

Unraveling the Li Penetration Mechanism in Polycrystalline Solid Electrolytes

The Stack Pressure Dilemma in Sulfide Electrolyte Based Li Metal Solid‐State Batteries: A Case Study with Li6PS5Cl Solid Electrolyte

Promises and Challenges of Next-Generation “Beyond Li-ion” Batteries for Electric Vehicles and Grid Decarbonization

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Product

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About

The Stack Pressure Dilemma in Sulfide Electrolyte Based Li Metal Solid‐State Batteries: A Case Study with Li₆PS₅Cl Solid Electrolyte