Cold sintering for Li1.5Al0.5Ge1.5(PO4)3 using LiNO3-LiOH as a transient solvent

Takashima, Kenji; Iwazaki, Yoshiki; Randall, Clive A.

doi:10.35848/1347-4065/ac33cf

Cited by 10 publications

(8 citation statements)

References 29 publications

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“…The preferential dissolution of lithium ions has been widely reported in lithium-based oxide systems. [13,17] This can lead to secondary phases that are detrimental to ionic conduction. [18] In our case, we propose that incongruent dissolution results in a phase transition for LLZO.…”

Section: Resultsmentioning

confidence: 99%

Cold Sintering Enables the Reprocessing of LLZO‐Based Composites

Lan,

Ghasemi,

Hall

et al. 2024

ChemSusChem

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All‐solid‐state batteries have the potential for enhanced safety and capacity over conventional lithium ion batteries, and are anticipated to dominate the energy storage industry. As such, strategies to enable recycling of the individual components are crucial to minimize waste and prevent health and environmental harm. Here, we use cold sintering to reprocess solid‐state composite electrolytes, specifically Mg and Sr doped Li7La3Zr2O12 with polypropylene carbonate (PPC) and lithium perchlorate (LLZO–PPC–LiClO4). The low sintering temperature allows co‐sintering of ceramics, polymers and lithium salts, leading to re‐densification of the composite structures with reprocessing. Reprocessed LLZO–PPC–LiClO4 exhibits densified microstructures with ionic conductivities exceeding 10−4 S/cm at room temperature after 5 recycling cycles. All‐solid‐state lithium batteries fabricated with reprocessed electrolytes exhibit a high discharge capacity of 168 mA h g−1 at 0.1 C, and retention of performance at 0.2 C for over 100 cycles. Life cycle assessment (LCA) suggests that the recycled electrolyte outperforms the pristine electrolyte process in all environmental impact categories, highlighting cold sintering is a promising technology for recycling electrolytes.

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Section: Resultsmentioning

confidence: 99%

Cold Sintering Enables the Reprocessing of LLZO‐Based Composites

Lan,

Ghasemi,

Hall

et al. 2024

ChemSusChem

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“…Recently, cold sintering has been used to sinter oxide-based electrolytes with good ionic conductivity. For example, NASICON structured electrolytes, such as Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) (Takashima et al, 2021) and Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) (Liu et al, 2019), were prepared by CSP at 120 °C. The sintered LATP pellet with a relative density of 93% showed a high ionic conductivity of 8.04 × 10 −5 S cm -1 at room temperature.…”

Section: Csp Of Composite Electrolytesmentioning

confidence: 99%

Cold sintering-enabled interface engineering of composites for solid-state batteries

et al. 2023

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The cold sintering process (CSP) is a low-temperature consolidation method used to fabricate materials and their composites by applying transient solvents and external pressure. In this mechano-chemical process, the local dissolution, solvent evaporation, and supersaturation of the solute lead to “solution-precipitation” for consolidating various materials to nearly full densification, mimicking the natural pressure solution creep. Because of the low processing temperature (<300°C), it can bridge the temperature gap between ceramics, metals, and polymers for co-sintering composites. Therefore, CSP provides a promising strategy of interface engineering to readily integrate high-processing temperature ceramic materials (e.g., active electrode materials, ceramic solid-state electrolytes) as “grains” and low-melting-point additives (e.g., polymer binders, lithium salts, or solid-state polymer electrolytes) as “grain boundaries.” In this minireview, the mechanisms of geomimetics CSP and energy dissipations are discussed and compared to other sintering technologies. Specifically, the sintering dynamics and various sintering aids/conditions methods are reviewed to assist the low energy consumption processes. We also discuss the CSP-enabled consolidation and interface engineering for composite electrodes, composite solid-state electrolytes, and multi-component laminated structure battery devices for high-performance solid-state batteries. We then conclude the present review with a perspective on future opportunities and challenges.

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“…The Cold Sintering Process (CSP) has attracted much attention because of the ability to densify at low temperatures between 100 °C to 300 °C for a number of important functional ceramics such as BaTiO 3 , [1][2][3][4][5] ZnO, [6][7][8][9][10][11] V 2 O 5 , [12][13][14] SnO, 15) Li 2 MoO 4 , 16,17) Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP), [18][19][20] Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP), 20) and β-alumina, 21) and (K, Na)NbO 3 (KNN). [22][23][24] Under conventional sintering conditions, these ceramics must be densified at significantly higher temperatures, so one major interest is the potential that CSP can provide an alternative route to a sustainable production process.…”

Section: Introductionmentioning

confidence: 99%

Impact of PTFE particle size in designing BaTiO₃ dielectric composites under the cold sintering process

Nunokawa

Takashima

Mizuno

et al. 2023

Jpn. J. Appl. Phys.

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The Cold Sintering Process (CSP) can provide opportunities to fabricate high-performance BaTiO3 dielectric composites with polymer materials that are typically difficult to impossible to co-process under a conventional sintering process. Therefore, we investigated the preparation process of BaTiO3 sintered body by CSP and integrated a well-dispersed intergranular polymer phase. In this study, we focused on preparing BaTiO3 and Polytetrafluoroethylene (PTFE) composites. We considered the importance of the particle size of the PTFE phase, and correlated the impact on the composite dielectric properties. Through fitting a general-mixing-law to the dielectric properties as a function of volume fraction, we could deduce more homogeneous composites obtained in using the 200 nm PTFE powders. In addition, the temperature dependent dielectric properties and field dependent conductivity of the composites was investigated. It was found that with the good dispersion of the PTFE can suppress the leakage current density in the dielectric composites.

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Cold sintering for Li_1.5Al_0.5Ge_1.5(PO₄)₃ using LiNO₃-LiOH as a transient solvent

Cited by 10 publications

References 29 publications

Cold Sintering Enables the Reprocessing of LLZO‐Based Composites

Cold Sintering Enables the Reprocessing of LLZO‐Based Composites

Cold sintering-enabled interface engineering of composites for solid-state batteries

Impact of PTFE particle size in designing BaTiO₃ dielectric composites under the cold sintering process

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Cold sintering for Li1.5Al0.5Ge1.5(PO4)3 using LiNO3-LiOH as a transient solvent

Cited by 10 publications

References 29 publications

Cold Sintering Enables the Reprocessing of LLZO‐Based Composites

Cold Sintering Enables the Reprocessing of LLZO‐Based Composites

Cold sintering-enabled interface engineering of composites for solid-state batteries

Impact of PTFE particle size in designing BaTiO3 dielectric composites under the cold sintering process

Contact Info

Product

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Cold sintering for Li_1.5Al_0.5Ge_1.5(PO₄)₃ using LiNO₃-LiOH as a transient solvent

Impact of PTFE particle size in designing BaTiO₃ dielectric composites under the cold sintering process