Preparation and characterization of glass solid electrolytes in the pseudoternary system Li 3 BO 3 -Li 2 SO 4 -Li 2 CO 3

Nagao, Kenji; Nose, Masashi; Kato, Akira; Sakuda, Atsushi; Hayashi, Akitoshi; Tatsumisago, Masahiro

doi:10.1016/j.ssi.2017.05.009

Cited by 41 publications

(22 citation statements)

References 36 publications

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“…However, the room temperature conductivity in as-deposited NASICON-type SE films by AD is reported to be only around 10 −6 S cm −1 [37,38]. Since the ceramic particles are plastically deformed and consolidated in the AD process, the use of oxide-based SE materials with both good Li + conduction property and deformability [50,51] is the key to form a better solid–solid interface in the composite electrode by AD. We are now trying to form a thicker composite electrode with LVO as an active material on LLZT by AD, and the progress will be reported in a forthcoming paper.…”

Section: Resultsmentioning

confidence: 99%

Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition

et al. 2018

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We fabricated lithium trivanadate LiV3O8 (LVO) film electrodes for the first time on a garnet-type Ta-doped Li7La3Zr2O12 (LLZT) solid electrolyte using the aerosol deposition (AD) method. Ball-milled LVO powder with sizes in the range of 0.5–2 µm was used as a raw material for LVO film fabrication via impact consolidation at room temperature. LVO film (thickness = 5 µm) formed by AD has a dense structure composed of deformed and fractured LVO particles and pores were not observed at the LVO/LLZT interface. For electrochemical characterization of LVO film electrodes, lithium (Li) metal foil was attached on the other end face of a LLZT pellet to comprise a LVO/LLZT/Li all-solid-state cell. From impedance measurements, the charge transfer resistance at the LVO/LLZT interface is estimated to be around 103 Ω cm2 at room temperature, which is much higher than at the Li/LLZT interface. Reversible charge and discharge reactions in the LVO/LLZT/Li cell were demonstrated and the specific capacities were 100 and 290 mAh g−1 at 50 and 100 °C. Good cycling stability of electrode reaction indicates strong adhesion between the LVO film electrode formed via impact consolidation and LLZT.

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Section: Resultsmentioning

confidence: 99%

Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition

et al. 2018

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“…12 In the case of a Li4SiO4-Li3PO4 system, when the ratio of Li4SiO4 to Li3PO4 is 1:3, a high Li-ion conductivity of 10 -3 S cm -1 has been recorded at 573 K. 10 A Li2CO3-Li3BO3-Li2SO4 ternary mixed system has also been reported as a promising system, although the combinatorial space experimentally explored had a limited area, and 10 -5 S cm -1 was recorded at room temperature. 13 The use of computer-aided material designs, without the need for experiments, has been flourishing because recent computational developments have made it possible to produce sufficient physical values through density functional theory (DFT) calculations. In particular, many new materials have recently been predicted through the effective combination of DFT calculations and machine learning.…”

Section: Introductionmentioning

confidence: 99%

Li-Ion Conductive Li3PO4-Li3BO3-Li2SO4 Mixture: Prevision through Density Functional Molecular Dynamics and Machine Learning

Sumita

Homma

Kaneta

et al. 2019

Bulletin of the Chemical Society of Japan

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The development of high Li-ion conductive solid electrolytes is crucial for the practical use of all solid-state Li-ion batteries. The mixing of hetero Li-ion conductive substances is a known method for enhancing the Li-ion conductivity more than in the original substances. In this study, using computer simulations, we proved that a ternary Li3PO4-Li3BO3-Li2SO4 system has the potential to demonstrate improved Li-ion conductivity based on the introduction of a quasi-Li/oxygen vacancy. The Li-ion conductivities of this ternary system were calculated using several model systems based on the density functional molecular dynamics under an isothermal-isobaric ensemble. However, an exploration using the density functional molecular dynamics cannot cover the entire combinatorial space owing to a lack of computational capability. To search through a vast combinatorial space, we conducted analyses using a machine learning technique. The analysis results clarify the relationship between Li-ion conductivity and phonon free energy, and allow the optimum composition ratio with the highest Li-ion conductivity to be predicted.

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“…We have reported the mechanochemical synthesis of sulfide and oxide glass electrolytes [2][3][4][5][6][7][8][9]. In particular, the Li3BO3-Li2SO4-Li2CO3 glass-ceramic electrolytes prepared by mechanical milling and consecutive heat treatment showed relatively high lithium ionic conductivity of 10 -6 -10 -5 S cm -1 at room temperature [6][7][8][9]. In addition, these oxide glass-ceramic electrolytes easily deform and large contact area with active materials can be achieved simply by pressing at room temperature.…”

Section: Introductionmentioning

confidence: 99%

Amorphous LiCoO2-based Positive Electrode Active Materials with Good Formability for All-Solid-State Rechargeable Batteries

et al. 2018

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Amorphous LiCoO2-based positive electrode materials are synthesized by a mechanical milling technique. As a lithium oxy-acid, Li2SO4, Li3PO4, Li3BO3, Li2CO3, and LiNO3 are selected and milled with LiCoO2. XRD patterns indicate that reaction between LiCoO2 and these lithium oxy-acids proceeds. Amorphization mainly occurs, and several broad peaks attributable to cubic LiCoO2 are observed in all the samples. These amorphous active materials show mixed conductivities of electron and lithium ion. All-solid-state cells using the prepared amorphous active materials and the Li2.9B0.9S0.1O3.1 glass-ceramic electrolyte are fabricated and their charge-discharge properties are examined. The cells with only the 80LiCoO2·20Li2SO4 (mol%) and the 80LiCoO2·20Li3PO4 active materials function as secondary batteries. This is because higher lithium ionic conductivities are obtained in the 80LiCoO2·20Li2SO4 and 80LiCoO2·20Li3PO4 active materials than in the others. The largest capacity is obtained in the cell with the 80LiCoO2·20Li2SO4 active material because of its good formability and high lithium ionic conductivity. In addition, the cell with the 80LiCoO2·20Li2SO4 positive electrode active material shows the better cycle and rate performance than that with the crystalline LiCoO2. It is noted that the amorphization with lithium oxy-acids is a promising technique for achieving a novel active material with better electrochemical performance.

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Preparation and characterization of glass solid electrolytes in the pseudoternary system Li 3 BO 3 -Li 2 SO 4 -Li 2 CO 3

Cited by 41 publications

References 36 publications

Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition

Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition

Li-Ion Conductive Li3PO4-Li3BO3-Li2SO4 Mixture: Prevision through Density Functional Molecular Dynamics and Machine Learning

Amorphous LiCoO2-based Positive Electrode Active Materials with Good Formability for All-Solid-State Rechargeable Batteries

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