Li–Garnet Solid-State Batteries with LLZO Scaffolds

Kravchyk, Kostiantyn V.; Zhang, Huanyu; Okur, Faruk; Kovalenko, Maksym V.

doi:10.1021/accountsmr.2c00004

Cited by 19 publications

(20 citation statements)

References 33 publications

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“…Since the discovery of Li 7 La 3 Zr 2 O 12 (LLZO) solid-state electrolytes (SSEs) and the realization of their high potential to replace combustible organic electrolytes in Li-ion batteries [1][2][3][4][5] and voids. [30][31][32][33][34][35] On the one hand, the formation of voids during stripping can be mitigated by the larger surface area of the LLZO/Li interface in the scaffold compared to dense LLZO ceramics. On the other hand, Li can be stored in the pores of the LLZO scaffold during Li deposition, thereby avoiding dynamic changes in cell volume.…”

Section: Introductionmentioning

confidence: 99%

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Okur

Zhang

Karabay

et al. 2023

Advanced Energy Materials

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While significant progress has been achieved in the field of Li‐garnet solid‐state batteries, their further development, is hindered by the formation of cavities at the Li7La3Zr2O12 (LLZO)/Li interface at practically relevant current densities and areal capacities exceeding 1 mA cm−2 and 1 mAh cm−2. As a result, the cells exhibit limited cycling stability due to the inhomogeneous distribution of the applied current density, and therefore, the formation of Li dendrites. Another aspect of high importance is associated with the development of the fabrication methodology of thin LLZO electrolytes for achieving the high energy density of Li‐garnet solid‐state batteries. To contribute to these two challenging problems, in this work, a facile intermediate‐stage sintering method of 50‐µm thin and porous LLZO membranes with a mean pore size of 2.5 µm is presented. The employment of such porous LLZO membranes not only provides an effective means of mitigating the formation of voids at the LLZO/Li interface due to the increased LLZO/Li surface area, but also maximizes achievable energy densities. It is demonstrated that fabricated porous LLZO membranes exhibit long cycling stability of over 1480 h at a current density of 0.5 mA cm−2.

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Section: Introductionmentioning

confidence: 99%

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Okur

Zhang

Karabay

et al. 2023

Advanced Energy Materials

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“…In the case of ZELMB‐s, the host structure is initially considered empty. [ 19 ] Accordingly, during Li deposition into the host, the cell volume and the VED remain constant until over‐plating occurs, where the deposited Li displaces an equivalent volume of solid electrolyte. Accordingly, during over‐plating, the cell volume increases and the VED decreases.…”

Section: Resultsmentioning

confidence: 99%

“…estimated the GED and VED of solid‐state batteries based on porous LLZO host structures for multi‐layer pouch cells. [ 19 ] They showed that trilayer‐structures reach VED of 975 Wh L −1 but GED below 275 Wh kg −1 , while bi‐layer structures achieve slightly higher GED of up to 285 Wh kg −1 . Bilayer structures with 20 µm dense plus 50 µm porous (70 %) layers have been shown to achieve 329 Wh kg −1 and 972 Wh L −1 .…”

Section: Resultsmentioning

confidence: 99%

Benchmarking and Critical Design Considerations of Zero‐Excess Li‐Metal Batteries

Lohrberg

Voigt

Maletti

et al. 2023

Adv Funct Materials

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Zero-excess Li metal batteries (ZELMBs), in which a Li-anode is formed in situ during charging, have received much attention in recent years. ZELMBs bear great potential to increase energy density and facilitate battery production, thereby reducing cost as well as material and energy consumption. Practical application of ZELMBs has so far been limited by challenges related to the non-uniform deposition behavior of Li, leading to inadequate performance and safety concerns. To address these issues, promising approaches have been developed in recent years, including modifications of the current collector, electrolyte, and cycling protocols. While these approaches improve the long-term stability of ZELMB, they also reduce the energy density by introducing inactive materials into the cell. Herein, critical design criteria for the various optimization approaches in ZELMB research are established. Nominal volumetric and gravimetric energy densities are determined based on the degree of modification. Thresholds are determined for each of the strategies at which the energy density gain of ZELMB vanishes compared to other cell configurations. These findings are compared to literature results to provide guidance for the further development of ZELMB.

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“…Briefly, the calculations were performed for a full cell consisting of a porous/dense LLZO membrane, and an NMC811 cathode with an areal capacity of 3 mAh cm −2 , as recently reported in our work (see ref. [44,45] for details). The anode side is designed to be anode-free.…”

Section: Electrochemical Characterizationmentioning

confidence: 99%

Bilayer Dense‐Porous Li₇La₃Zr₂O₁₂ Membranes for High‐Performance Li‐Garnet Solid‐State Batteries

et al. 2023

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Li dendrites form inLi 7 La 3 Zr 2 O 12 (LLZO) solid electrolytes due to intrinsic volume changes of Li and the appearance of voids at the Li metal/LLZO interface. Bilayer dense-porous LLZO membranes make for a compelling solution of this pertinent challenge in the field of Li-garnet solid-state batteries (SSB). Lithium is thus stored in the pores of the LLZO, thereby avoiding i) dynamic changes of the anode volume and ii) the formation of voids during Li stripping due to increased surface area of the Li/LLZO interface. The dense layer then additionally reduces the probability of short circuits during cell charging. In this work, a method for producing such bilayer membranes utilizing sequential tape-casting of porous and dense layers is reported. The minimum attainable thicknesses are 8-10 μm for dense and 32-35 μm for porous layers, enabling gravimetric and volumetric energy densities of Li-garnet SSBs of 279 Wh kg −1 and 1003 Wh L −1 , respectively. Bilayer LLZO membranes in symmetrical cell configuration exhibit high critical current density up to 6 mA cm −2 and cycling stability of over 160 cycles at a current density of 0.5 mA cm −2 at an areal capacity limitation of 0.25 mAh cm −2 .

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Li–Garnet Solid-State Batteries with LLZO Scaffolds

Abstract: Parameters for energy density calculations, charging process schematics, calculated gravimetric and volumetric energy densities, calculated current densities vs pore sizes (PDF)

Cited by 19 publications

References 33 publications

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Benchmarking and Critical Design Considerations of Zero‐Excess Li‐Metal Batteries

Bilayer Dense‐Porous Li₇La₃Zr₂O₁₂ Membranes for High‐Performance Li‐Garnet Solid‐State Batteries

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Li–Garnet Solid-State Batteries with LLZO Scaffolds

Abstract: Parameters for energy density calculations, charging process schematics, calculated gravimetric and volumetric energy densities, calculated current densities vs pore sizes (PDF)

Cited by 19 publications

References 33 publications

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Intermediate‐Stage Sintered LLZO Scaffolds for Li‐Garnet Solid‐State Batteries

Benchmarking and Critical Design Considerations of Zero‐Excess Li‐Metal Batteries

Bilayer Dense‐Porous Li7La3Zr2O12 Membranes for High‐Performance Li‐Garnet Solid‐State Batteries

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Bilayer Dense‐Porous Li₇La₃Zr₂O₁₂ Membranes for High‐Performance Li‐Garnet Solid‐State Batteries