Dense freeze‐cast Li7La3Zr2O12 solid electrolytes with oriented open porosity and contiguous ceramic scaffold

Buannic, Lucienne; Naviroj, Maninpat; Miller, Steve; Zagórski, Jakub; Faber, K. T.; Llordés, Anna

doi:10.1111/jace.15938

Cited by 31 publications

(14 citation statements)

References 35 publications

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“…The pellets derived from conventional sol-gel and electrospinning possess more pores and voids than the pellets derived from the melt-spun bers. 16,19,[23][24][25][26][27][28][29] In general, the particles sintering involves neck formation, mass transport and pore closure, with the major driving force being the reduction of total surface energy. Nanoparticles exhibit a large surface-to-volume ratio with high surface energy, which implies that the sintering of nanoparticles should yield high-density pellets due to the presence of a large driving force.…”

Section: Resultsmentioning

confidence: 99%

A facile and scalable process to synthesize flexible lithium ion conductive glass-ceramic fibers

Xie

et al. 2019

RSC Adv.

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Section: Resultsmentioning

confidence: 99%

A facile and scalable process to synthesize flexible lithium ion conductive glass-ceramic fibers

Xie

et al. 2019

RSC Adv.

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“…[32,33] To achieve desired porous structure with a pure crystalline phase, conventional sintering methods typically rely on poreforming agent [32] or freeze casting. [29,34,35] In particular, these conventional approaches to sinter porous ceramics can take advantage of prolonged sintering time at relatively low temperatures. In this low-temperature kinetic region, surface diffusion, which has a low activation energy, controls and leads to neck forming (bonding) without densification, yet surface diffusion also promotes grain growth (coarsening).…”

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confidence: 99%

High‐Temperature Ultrafast Sintering: Exploiting a New Kinetic Region to Fabricate Porous Solid‐State Electrolyte Scaffolds

et al. 2021

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issue has greatly hindered the development of these technologies for broader applications. [5,6] Solid-state electrolytes (SSEs) represent one promising solution to this problem as they offer better safety and potentially higher volumetric energy density. [7][8][9][10][11] A range of SSEs materials have been explored so far, with polymers [12,13] and ceramic Li-ion conductors [14] being the leading contenders. Among them, polymer SSEs show seamless interfacial contact and relatively larger production scale, [15] but suffer from low mechanical strength [16] and poor thermal stability. In addition, the organic backbone of these materials does not fundamentally address the flammability issue and is prone to thermal runaway. In comparison, ceramic Li-ion conductors such as garnet, [17,18] LISICON Li 10 GeP 2 S 12 , [19] and so on exhibit better mechanical strength and Li-ion conductivity, but comes with an expense of processability, poor interfacial contact, and flexibility. [20,21] Despite the high promise and broad research interest, these problems continue to limit the practicality of ceramic SSEs for broader applications. [22,23] It has been shown that integrating ceramic and polymer SSEs together promises a viable route to harvest the merits of the two while neutralizing each other's drawbacks. [6,[24][25][26] Such a "polymer in ceramic" strategy often requires the synthesis of 3D porous ceramic scaffold to form continuous Li-ion transport pathways with polymer SSEs. [27][28][29] On the other hand, the porous ceramic scaffold can also be used to decrease the interfacial resistance between the electrolyte and Li metal anode, [30] conventional intercalation cathode, [31] or conversion cathode such as sulfur. [32,33] To achieve desired porous structure with a pure crystalline phase, conventional sintering methods typically rely on poreforming agent [32] or freeze casting. [29,34,35] In particular, these conventional approaches to sinter porous ceramics can take advantage of prolonged sintering time at relatively low temperatures. In this low-temperature kinetic region, surface diffusion, which has a low activation energy, controls and leads to neck forming (bonding) without densification, yet surface diffusion also promotes grain growth (coarsening). The long sintering time also causes significant Li loss due to its highly volatile nature, which deteriorates the quality of the porous Solid-state batteries (SSBs) promise better safety and potentially higher energy density than the conventional liquid-or gel-based ones. In practice, the implementation of SSBs often necessitates 3D porous scaffolds made by ceramic solid-state electrolytes (SSEs). Herein, a general and facile method to sinter 3D porous scaffolds with a range of ceramic SSEs on various substrates at high temperature in seconds is reported. The high temperature enables rapid reactive sintering toward the desired crystalline phase and expedites the surface diffusion of grains for neck growth; meanwhile, the short sintering duration limits the coarsening, ...

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“…Apart from the 3D bilayer, another nanostructured LLZO was synthesized via template methods, 87 3D-printer, 108 and freeze-casting. [111][112][113] The scaffold structure also shows promising potential for a corporation with metal oxides. On the basis of screen printing, an LCO/garnet composite cathode delivered a high utilization of active material (81%) at 0.1 C. 114 However, in most of these designs, an ionic liquid electrolyte was added to wet the cathode side interface.…”

Section: Toward To Cathode/garnet Electrolyte Interfacementioning

confidence: 99%

Progress and perspective of interface design in garnet electrolyte‐based all‐solid‐state batteries

et al. 2021

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Inorganic solid-state electrolytes (SSEs) are nonflammable alternatives to the commercial liquid-phase electrolytes. This enables the use of lithium (Li) metal as an anode, providing high-energy density and improved stability by avoiding unwanted liquid-phase chemical reactions. Among the different types of SSEs, the garnet-type electrolytes witness a rapid development and are considered as one of the top candidates to pair with Li metal due to their high ionic conductivity, thermal, and electrochemical stability. However, the large resistances at the interface between garnet-type electrolytes and cathode/anode are the major bottlenecks for delivering desirable electrochemical performances of all-solid-state batteries (SSBs). The electrolyte/anode interface also suffers from metallic dendrite formation, leading to rapid performance degradation. This is a fundamental material challenge due to the poor contact and wettability between garnet-type electrolytes with electrode materials. Here, we summarize and analyze the recent contributions in mitigating such materials challenges at the interface. Strategies used to address these challenges are divided into different categories with regard to their working principles. On one hand, progress has been made in the anode/ garnet interface, such as the successful application of Li-alloy anode and different artificial interlayers, significantly improving interfacial performance. On the other hand, the desired cathode/garnet interface is still hard to reach due to the complex chemical and physical structure at the cathode. The common methods used are nanostructured cathode host and sintering additives for increasing the contact area.On the basis of this information, we present our views on the remaining challenges and future research of electrode/garnet interface. This review not only motivates the need for further understanding of the fundamentals, stability, and modifications of the garnet/electrode interfaces but also provides guidelines for the future design of the interface for SSB.

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Dense freeze‐cast Li₇La₃Zr₂O₁₂ solid electrolytes with oriented open porosity and contiguous ceramic scaffold

Cited by 31 publications

References 35 publications

A facile and scalable process to synthesize flexible lithium ion conductive glass-ceramic fibers

A facile and scalable process to synthesize flexible lithium ion conductive glass-ceramic fibers

High‐Temperature Ultrafast Sintering: Exploiting a New Kinetic Region to Fabricate Porous Solid‐State Electrolyte Scaffolds

Progress and perspective of interface design in garnet electrolyte‐based all‐solid‐state batteries

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