Mechanochemical synthesis of Li-argyrodite Li6PS5X (X=Cl, Br, I) as sulfur-based solid electrolytes for all solid state batteries application

Boulineau, Sylvain; Courty, Matthieu; Tarascon, Jean‐Marie; Viallet, V.

doi:10.1016/j.ssi.2012.06.008

Cited by 412 publications

(389 citation statements)

References 12 publications

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“…The mechanical milling was performed using a planetary ball mill with a zirconia pot with 0.5 g of sample and 10 mm diameter zirconia balls (15 balls) at 600 rpm for 40 h [ 6,16 ]. The as synthetized Li PS Cl powder was then dissolved in anhydrous ethanol (Wako Pure Chemicals, 99.5%).…”

Section: Methodsmentioning

confidence: 99%

“…The XRD pattern of the as synthetized Li PS Cl solid electrolyte prepared by mechanical milling shows broad peak characteristic of the argyrodite crystal phase [ 16,17,18 ] and additional peaks attributed to the un reacted Li S phase. The XRD patterns of Li PS Cl crystals after dissolution reprecipitation procedure, with and without binder, show sharper peaks than those of Li PS Cl obtained by mechanical milling, confirming a higher crystallinity after dissolution reprecipitation procedure.…”

Section: Methodsmentioning

confidence: 99%

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Effect of the binder content on the electrochemical performance of composite cathode using Li6PS5Cl precursor solution in an all-solid-state lithium battery

Rosero-Navarro

Kinoshita

Miura

et al. 2017

Ionics

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All solid state batteries with cathode composites containing high concentration of active materials are required to achieve higher energy densities. Here, a composite cathode containing up to 89 wt% of high voltage cathode active material (LiNi Mn Co O ) was prepared by covering this with a solution derived solid electrolyte (argyrodite, Li PS Cl) and the incorporation of different content binder (ethyl cellulose). All solid state batteries were fabricated using 80Li S•20P S (mol%) glass and indium metal as a solid electrolyte and anode, respectively. The all solid state battery with a composite cathode containing 0.5 wt% of ethyl cellulose showed an initial discharge capacity of 45 mAhg at 25 °C and maintained 91.7% of the discharge capacity after ten cycles, around 30% higher than that obtained for the battery with the composite cathode without a binder.

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Section: Methodsmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Effect of the binder content on the electrochemical performance of composite cathode using Li6PS5Cl precursor solution in an all-solid-state lithium battery

Rosero-Navarro

Kinoshita

Miura

et al. 2017

Ionics

View full text Add to dashboard Cite

show abstract

“…Studies investigating new electrolytes with much higher conductivity are in progress. Several crystals, such as Li10SnP2S12 (Boron et al, 2013) and Li6PS5Cl (Boulineau et al, 2012), have high conductivity of more than 10 −3 S cm…”

Section: Conductivitymentioning

confidence: 99%

Development of Sulfide Solid Electrolytes and Interface Formation Processes for Bulk-Type All-Solid-State Li and Na Batteries

2016

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All-solid-state batteries with inorganic solid electrolytes (SEs) are recognized as an ultimate goal of rechargeable batteries because of their high safety, versatile geometry, and good cycle life. Compared with thin-film batteries, increasing the reversible capacity of bulk-type all-solid-state batteries using electrode active material particles is difficult because contact areas at solid-solid interfaces between the electrode and electrolyte particles are limited. Sulfide SEs have several advantages of high conductivity, wide electrochemical window, and appropriate mechanical properties, such as formability, processability, and elastic modulus. Sulfide electrolyte with Li7P3S11 crystal has a high Li + ion conductivity of 1.7 × 10 −2 S cm −1 at 25°C. It is far beyond the Li + ion conductivity of conventional organic liquid electrolytes. The Na + ion conductivity of 7.4 × 10 −4 S cmis achieved for Na3.06P0.94Si0.06S4 with cubic structure. Moreover, formation of favorable solid-solid interfaces between electrode and electrolyte is important for realizing solid-state batteries. Sulfide electrolytes have better formability than oxide electrolytes. Consequently, a dense electrolyte separator and closely attached interfaces with active material particles are achieved via "room-temperature sintering" of sulfides merely by cold pressing without heat treatment. Elastic moduli for sulfide electrolytes are smaller than that of oxide electrolytes, and Na2S-P2S5 glass electrolytes have smaller Young's modulus than Li2S-P2S5 electrolytes. Cross-sectional SEM observations for a positive electrode layer reveal that sulfide electrolyte coating on active material particles increases interface areas even with a minimum volume of electrolyte, indicating that the energy density of bulk-type solid-state batteries is enhanced. Both surface coating of electrode particles and preparation of nanocomposite are effective for increasing the reversible capacity of the batteries. Our approaches to form solid-solid interfaces are demonstrated.

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“…The ionic conductivity of a Li 10 GeP 2 S 12 crystal, in particular, is 1.2 × 10 −2 S/cm (Kamaya et al, 2011). Argyrodite-type crystals with the stoichiometry Li 6 PS 5 X (X = Cl, Br, or I) also have high ionic conductivity (>10 −3 S/cm) (Deiseroth et al, 2008;Rao and Adams, 2011;Boulineau et al, 2012). In addition, the conductivities of some glasses, including 30Li 2 S-26B 2 S 3 -44LiI (Wada et al, 1983), 50Li 2 S-17P 2 S 5 -33LiBH 4 (Yamauchi et al, 2013), and 63Li 2 S-36SiS 2 -1Li 3 PO 4 (Aotani et al, 1994), have been reported to be as high as 1.5-1.7 × 10 −3 S/cm.…”

Section: Introductionmentioning

confidence: 99%

Structure and Ionic Conductivity of Li2S–P2S5 Glass Electrolytes Simulated with First-Principles Molecular Dynamics

Baba

Kawamura

2016

Front. Energy Res.

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Lithium thiophosphate-based materials are attractive as solid electrolytes in all-solidstate lithium batteries because glass or glass-ceramic structures of these materials are associated with very high conductivity. In this work, we modeled lithium thiophosphates with amorphous structures and investigated Li + mobilities by using molecular dynamics calculations based on density functional theory (DFT-MD). The structures of xLi 2 S-(100 − x)P 2 S 5 (x = 67, 70, 75, and 80) were created by randomly identifying appropriate compositions of Li + , PS The implication is that these amorphous structures are metastable. There was good agreement between calculated and experimental structure factors determined from X-ray scattering. The differences between the structure factors of amorphous structures were small, except for the first sharp diffraction peak, which was affected by the environment between Li and S atoms. Li + diffusion coefficients obtained from DFT-MD calculations at various temperatures for picosecond simulation times were on the order of 10 −3 -10 −5 Å 2 /ps. Ionic conductivities evaluated by the Nernst-Einstein relationship at 298.15 K were on the order of 10 −5 S/cm. The ionic conductivity of the amorphous structure with x = 75 was the highest among the amorphous structures because there was a balance between the number density and diffusibility of Li + . The simulations also suggested that isolated S atoms suppress Li + migration.

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Mechanochemical synthesis of Li-argyrodite Li6PS5X (X=Cl, Br, I) as sulfur-based solid electrolytes for all solid state batteries application

Cited by 412 publications

References 12 publications

Effect of the binder content on the electrochemical performance of composite cathode using Li6PS5Cl precursor solution in an all-solid-state lithium battery

Effect of the binder content on the electrochemical performance of composite cathode using Li6PS5Cl precursor solution in an all-solid-state lithium battery

Development of Sulfide Solid Electrolytes and Interface Formation Processes for Bulk-Type All-Solid-State Li and Na Batteries

Structure and Ionic Conductivity of Li2S–P2S5 Glass Electrolytes Simulated with First-Principles Molecular Dynamics

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