Rock-salt-type lithium metal sulphides as novel positive-electrode materials

Sakuda, Atsushi; Takeuchi, Tomonari; Okamura, Keisuke; Kobayashi, Hironori; Sakaebe, Hikarí; Tatsumi, Kuniaki; Ogumi, Zempachi

doi:10.1038/srep04883

Cited by 77 publications

(106 citation statements)

References 19 publications

(25 reference statements)

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“…The reversible capacity per unit area was 3.54 mAh cm . Rock-salt Li3NbS4 has been reported to exhibit reversible charging and discharging for compositions ranging between Li0.4NbS4 and Li3.9NbS4 when charged and discharged with cutoff voltages of 3.0 and 1.5 V (vs. Li + /Li), respectively (Sakuda et al, 2014c). Thus, Li3NbS4 can be used in all-solid-state cells as well as in the cells with carbonate-based liquid electrolytes.…”

Section: Methodsmentioning

confidence: 99%

High Reversibility of “Soft” Electrode Materials in All-Solid-State Batteries

Sakuda¹,

Takeuchi²,

Shikano³

et al. 2016

Front. Energy Res.

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All-solid-state batteries using inorganic solid electrolytes (SEs) are considered to be ideal batteries for electric vehicles and plug-in hybrid electric vehicles because they are potentially safer than conventional lithium-ion batteries (LIBs). In addition, all-solid-state batteries are expected to have long battery life owing to the inhibition of chemical side reactions because only lithium ions move through the typically used inorganic SEs. The development of high-energy density (more than 300 Wh kg −1 ) secondary batteries has been eagerly anticipated for years. The application of high-capacity electrode active materials is essential for fabricating such batteries. Recently, we proposed metal polysulfides as new electrode materials. These materials show higher conductivity and density than sulfur, which is advantageous for fabricating batteries with relatively higher energy density. Lithium niobium sulfides, such as Li3NbS4, have relatively high density, conductivity, and rate capability among metal polysulfide materials, and batteries with these materials have capacities high enough to potentially exceed the gravimetric-energy density of conventional LIBs. Favorable solid-solid contact between the electrode and electrolyte particles is a key factor for fabricating high performance all-solid-state batteries. Conventional oxide-based positive electrode materials tend to give rise to cracks during fabrication and/or charge-discharge processes. Here, we report all-solid-state cells using lithium niobium sulfide as a positive electrode material, where favorable solid-solid contact was established by using lithium sulfide electrode materials because of their high processability. Cracks were barely observed in the electrode particles in the all-solid-state cells before or after charging and discharging with a high capacity of approximately 400 mAh g −1 suggesting that the lithium niobium sulfide electrode charged and discharged without experiencing substantial mechanical damage. As a result, the all-solid-state cells retained more than 90% of their initial capacity after 200 cycles of charging and discharging at 0.5 mA cm −2 .

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Section: Methodsmentioning

confidence: 99%

High Reversibility of “Soft” Electrode Materials in All-Solid-State Batteries

Sakuda¹,

Takeuchi²,

Shikano³

et al. 2016

Front. Energy Res.

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“…These results are in agreement with our previous reports. [14][15][16][17] The prepared samples containing tin also charged and discharged, although their charge-discharge capacities gradually decreased as the tin ratio increased. Notably, the capacity was not proportional to the niobium content.…”

Section: ¹1mentioning

confidence: 99%

“…[8][9][10] We recently obtained lithium titanium sulfide, Li 2 TiS 3 , and lithium niobium sulfide, Li 3 NbS 4 , which had a cubic rocksalt structure, and their solid solutions, which were prepared by mechanochemical synthesis. [14][15][16][17] The lithium transition metal sulfides of cubic Li 2 TiS 3 and Li 3 NbS 4 can be used as electrode active materials for secondary batteries and exhibit high reversible capacities of 400 mAh g ¹1 . Mechanochemical synthesis has an attractive advantage that it is possible to obtain the product in a metastable state, such as materials with amorphous or highly symmetrical crystal structures.…”

Section: Introductionmentioning

confidence: 99%

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Cubic Rocksalt Li2SnS3 and a Solid Solution with Li3NbS4 Prepared by Mechanochemical Synthesis

et al. 2017

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“…Finally, taking into account the facile oxidation of Ti 3+ during the sputtering process and the perfect reversibility of the anion-based redox process, the preparation of thin electrodes from Li 2 S-TiS 2 target compositions appears as a promising prospect. 46 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 …”

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Dual Cation- and Anion-Based Redox Process in Lithium Titanium Oxysulfide Thin Film Cathodes for All-Solid-State Lithium-Ion Batteries

Dubois

Pecquenard

Soulé

et al. 2017

ACS Appl. Mater. Interfaces

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Abstract:A dual redox process involving Ti 3+ /Ti 4+ cation species and S 2-/(S 2 ) 2-anion species is highlighted in oxygenated lithium titanium sulfide thin film electrodes during lithium (de)insertion, leading to a high specific capacity. These cathodes for all-solid-state lithium-ion microbatteries are synthesized by sputtering of LiTiS 2 targets prepared by different means. The limited oxygenation of the films that is induced during the sputtering process favors the occurrence of the S 2-/(S 2 ) 2-redox process at the expense of the Ti 3+ /Ti 4+ one during the battery operation, and influences its voltage profile. Finally, a perfect reversibility of both electrochemical processes is observed, whatever the initial film composition. All-solid-state lithium microbatteries using these amorphous lithiated titanium disulfide thin films and operated between 1.5-3.0 V/Li + /Li deliver a greater capacity (210-270 mAh g -1 ) than LiCoO 2 , with a perfect capacity retention (-0.0015 % cycle -1 ).

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Rock-salt-type lithium metal sulphides as novel positive-electrode materials

Cited by 77 publications

References 19 publications

High Reversibility of “Soft” Electrode Materials in All-Solid-State Batteries

High Reversibility of “Soft” Electrode Materials in All-Solid-State Batteries

Cubic Rocksalt Li<sub>2</sub>SnS<sub>3</sub> and a Solid Solution with Li<sub>3</sub>NbS<sub>4</sub> Prepared by Mechanochemical Synthesis

Dual Cation- and Anion-Based Redox Process in Lithium Titanium Oxysulfide Thin Film Cathodes for All-Solid-State Lithium-Ion Batteries

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