Microstructure and properties investigation of garnet structured Li7La3Zr2O12 as electrolyte for all-solid-state batteries

Nonemacher, Juliane Franciele; Hüter, Claas; Zheng, Hao; Malzbender, Jürgen; Krüger, Manja; Spatschek, Robert; Finsterbusch, Martin

doi:10.1016/j.ssi.2018.04.016

Cited by 35 publications

(28 citation statements)

References 46 publications

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“…The rather low values of the elastic modulus and hardness of high‐density LLZO specimens compared to those of other types of Li oxides, usually reflected in the fracture toughness, can be advantageous in terms of manufacturing, yet the large scattering needs to be addressed. [ 119 ] A mixing of the electrolyte with one or two of the electrodes is considered vital to maintain intimate contact and minimize ohmic resistance during prolonged battery operation.…”

Section: Solid Electrolytes: Sulfides and Oxidesmentioning

confidence: 99%

“…[119] The large variation in the Young's modulus, even at high relative densities of LLZO, is a manufacturing limitation, especially as it can echo fracture toughness values and unforeseen battery failure. [119] Doped LLZO has been established as a material with isotropic elastic properties, as indicated by the Zener anisotropy ratio A of ≈1.3 for the cubic crystal (note that, A = 1 refers to an isotropic material). [137] In isotropic elastic solids, the bulk modulus B and shear modulus G are correlated to the Young's modulus by the Poisson ratio ν [275] (ν Ta = 0.24 and ν Al = 0.26 for Ta-and Al-doped LLZO, respectively).…”

Section: Oxidesmentioning

confidence: 99%

“…[177] Densification of LLZO solid-electrolyte powders with low porosity is of utmost importance for optimization and unification of the mechanical and electrical properties. [119,178] Nevertheless, achieving a dense electrolyte with the right phase is crucial to improve the ionic conductivity. For example, the total ionic conductivity of cubic LLZO (Li 6.19 Al 0.27 La 3 Zr 2 O 12 ) can change by more than an order of magnitude from 0.009 to 0.34 × 10 −3 S cm −1 , changing the relative theoretical density from 85% to 98%, respectively.…”

Section: Oxidesmentioning

confidence: 99%

“…have already equated or surpassed those of their liquid counterparts (≈10 −2 -10 −1 S cm −1 ). [40,78,255] Currently, only scarce literature data is available on the mechanical integrity of garnet-type LLZO [119,137,[178][179][180][181][256][257][258] and sulfide-type LPS [149][150][151]155,259] and LGPS [77,171,260,261] (Figure 3). During the operation of a solidstate battery, the contraction and expansion of the active material of the electrode during intercalation and deintercalation of Li + ions induces the formation of internal stress within the electrode structure and may lead to volume changes, [262][263][264][265] poor interfacial contact toward the electrolyte being a solid, and fewer percolation pathways for Li diffusion due to fragmentation of the electrodes.…”

Section: Mechanical Stability and Processabilitymentioning

confidence: 99%

“…[178,257,275,289] Cubic Ta-doped LLZO (relative density 92%-98%) exhibited large scatter in the single-crystal hardness, ranging from ≈9-12 GPa (the large scatter was related to surface roughness); however, once considering microstructure features, the effective hardness was unified at ≈5-6 GPa. [119] Recently, the microscopic/local hardness of LLZO was assessed using the micro-pillar indentation splitting method and was determined to be ≈8.5 GPa (with a fracture toughness of 0.99 MPa m 1/2 ). [181] The hardness values of LLZO, LLTO, and LATP indicate reduced plastic deformation in all three types of Li oxides, which in turn leads to extremely brittle behavior.…”

Section: Oxidesmentioning

confidence: 99%

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Solid‐State Li–Metal Batteries: Challenges and Horizons of Oxide and Sulfide Solid Electrolytes and Their Interfaces

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lightweight, and compact and allow for versatile device geometries. They must also be scalable and offer high energy density to provide improved packing efficiency and longer device operation. Although both Ni-MH batteries and LIBs have been commercialized since the 1990s, [1] LIBs possess twice the gravimetric/volumetric energy density (250 Wh kg −1 /700 Wh L −1 vs 170 Wh kg −1 /350 Wh L −1 ), [2] higher battery voltage (3.7 V vs 1.2 V), and longer cycle life with lower self-discharge, [3] contributing tremendously to the proliferation of portable electronic devices (e.g., mobile phones, laptops, cameras, tablets) as well as emerging new technologies such as wearable electronic devices (e.g., smart watches and sport-related tracking devices). Their high gravimetric/ volumetric energy density, [2] excellent cycle life (thousands of cycles), and lack of the memory effect have positioned LIBs as state-of-the-art power sources and one of the greatest successes of modern electrochemistry, revolutionizing the way we acquire, process, transmit, and share information globally. Nevertheless, advances in battery energy density, safety, costs, and flexibility in shape and size are still needed to keep up with the rapidly growing demand for devices with even longer runtime as well as real-time data collection and transmission capabilities in addition to increasingly energy-demanding applications such as electric vehicles (EVs) and electricity grid storage. Even though LIBs were first commercialized in all electric vehicles (EVs) in 2010 and also emerged for grid application in the same time frame, the low energy density (≈250 Wh kg −1 ) and high average cost (≈$156 kWh −1 in 2019) of conventional LIBs do not meet the requirements for advanced EVs and grid-scale energy storage. [4][5][6] Specifically, the driving range per charge (miles), which is related to the energy density of each cell, and the cost are important parameters for EVs. For example, one 85 kWh battery pack in a Tesla Model S requires 7104 LIB cells, with an energy density of 265 Wh kg −1 , providing an average range of 250 miles, which is ahead of the range of other EVs but still behind the target of 375 miles. [4] In grid-scale applications, LIBs can be used for various tasks: frequency regulation, peak shaving, load leveling, and large-scale integration of renewable energies, with specific properties generally required for each task. For frequency regulation, LIBs need to provide a fast response, high rate performance, and high-power capability,The introduction of new, safe, and reliable solid-electrolyte chemistries and technologies can potentially overcome the challenges facing their liquid counterparts while widening the breadth of possible applications. Through tech-historic evolution and rationally analyzing the transition from liquidbased Li-ion batteries (LIBs) to all-solid-state Li-metal batteries (ASSLBs), a roadmap for the development of a successful oxide and sulfide-based ASSLB focusing on interfacial challenges is introduced, while accounting ...

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Section: Solid Electrolytes: Sulfides and Oxidesmentioning

confidence: 99%

Section: Oxidesmentioning

confidence: 99%

Section: Oxidesmentioning

confidence: 99%

Section: Mechanical Stability and Processabilitymentioning

confidence: 99%

Section: Oxidesmentioning

confidence: 99%

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Solid‐State Li–Metal Batteries: Challenges and Horizons of Oxide and Sulfide Solid Electrolytes and Their Interfaces

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Shape Persistent, Highly Conductive Ionogels from Ionic Liquids Reinforced with Cellulose Nanocrystal Network

Lee

Erwin

Buxton

et al. 2021

Adv Funct Materials

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Shape-persistent, conductive ionogels where both mechanical strength and ionic conductivity are enhanced are developed using multiphase materials composed of cellulose nanocrystals and hyperbranched polymeric ionic liquids (PILs) as a mechanically strong supporting network matrix for ionic liquids with an interrupted ion-conducting pathway. The integration of needlelike nanocrystals and PIL promotes the formation of multiple hydrogen bonding and electrostatic ionic interaction capacitance, resulting in the formation of interconnected networks capable of confining a high amount of ionic liquid (≈95 wt%) without losing its self-sustained shape. The resulting nanoporous and robust ionogels possess outstanding mechanical strength with a high compressive elastic modulus (≈5.6 MPa), comparable to that of tough, rubbery materials. Surprisingly, these rigid materials preserve the high ionic conductivity of original ionic liquids (≈7.8 mS cm −1 ), which are distributed within and supported by the nanocrystal network-like rigid frame. On the one hand, such stable materials possess superior ionic conductivities in comparison to traditional solid electrolytes; on the other hand, the high compression resistance and shapepersistence allow for easy handling in comparison to traditional fluidic electrolytes. The synergistic enhancement in ion transport and solid-like mechanical properties afforded by these ionogel materials make them intriguing candidates for sustainable electrodeless energy storage and harvesting matrices.

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Abnormal Ionic Conductivities in Halide NaBi₃O₄Cl₂ Induced by Absorbing Water and a Derived Oxhydryl Group

Sun

Plewa

et al. 2020

Angewandte Chemie

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In hunting for safe and cost‐effective materials for post‐Li‐ion energy storage, the design and synthesis of high‐performance solid electrolytes (SEs) for all‐solid‐state batteries are bottlenecks. Many issues associated with chemical stability during processing and storage and use of the SEs in ambient conditions need to be addressed. Now, the effect of water as well as oxyhdryl group (.OH) on NaBi3O4Cl2 are investigated by evaluating ionic conductivity. The presence of water and .OH results in an increase in ionic conductivity of NaBi3O4Cl2 owing to diffusion of H2O into NaBi3O4Cl2, partially forming binding .OH through oxygen vacancy repairing. Ab initio calculations reveal that the electrons significantly accumulate around .OH and induce a more negative charge center, which can promote Na+ hopping. This finding is fundamental for understanding the essential role of H2O in halide‐based SEs and provides possible roles in designing water‐insensitive SEs through control of defects.

show abstract

Microstructure and properties investigation of garnet structured Li7La3Zr2O12 as electrolyte for all-solid-state batteries

Cited by 35 publications

References 46 publications

Solid‐State Li–Metal Batteries: Challenges and Horizons of Oxide and Sulfide Solid Electrolytes and Their Interfaces

Solid‐State Li–Metal Batteries: Challenges and Horizons of Oxide and Sulfide Solid Electrolytes and Their Interfaces

Shape Persistent, Highly Conductive Ionogels from Ionic Liquids Reinforced with Cellulose Nanocrystal Network

Abnormal Ionic Conductivities in Halide NaBi₃O₄Cl₂ Induced by Absorbing Water and a Derived Oxhydryl Group

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Microstructure and properties investigation of garnet structured Li7La3Zr2O12 as electrolyte for all-solid-state batteries

Cited by 35 publications

References 46 publications

Solid‐State Li–Metal Batteries: Challenges and Horizons of Oxide and Sulfide Solid Electrolytes and Their Interfaces

Solid‐State Li–Metal Batteries: Challenges and Horizons of Oxide and Sulfide Solid Electrolytes and Their Interfaces

Shape Persistent, Highly Conductive Ionogels from Ionic Liquids Reinforced with Cellulose Nanocrystal Network

Abnormal Ionic Conductivities in Halide NaBi3O4Cl2 Induced by Absorbing Water and a Derived Oxhydryl Group

Contact Info

Product

Resources

About

Abnormal Ionic Conductivities in Halide NaBi₃O₄Cl₂ Induced by Absorbing Water and a Derived Oxhydryl Group