JP2010113820A - Lithium ion conductive solid electrolyte composition and battery using it - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a composition with excellent processibility by retaining solid electrolyte while maintaining ion conductivity. <P>SOLUTION: The composition contains lithium ion conductive solid electrolyte consisting of at least a kind or more elements selected from phosphorus, silicon, germanium, and boron; and a kind or more compounds selected from a carbonate compound expressed in: R<SB>1</SB>-O-C(=O)-O-R<SB>2</SB>(in the formula, R<SB>1</SB>, R<SB>2</SB>denote a group with the carbon number of 2 or more, respectively); an ether compound expressed in: R<SB>3</SB>-O-R<SB>4</SB>-O-R<SB>5</SB>(in the formula, R<SB>3</SB>and R<SB>5</SB>denote a group with the carbon number of 2 or more, and R<SB>4</SB>denotes a group with the carbon number of 1 or more); and a nitrile compound expressed in R<SB>6</SB>-CN (in the formula, R<SB>6</SB>denotes a group with the carbon number of 2 or more). <P>COPYRIGHT: (C)2010,JPO&INPIT

Description

  The present invention relates to a lithium ion conductive electrolyte composition and a lithium battery using the same.

In recent years, the demand for secondary batteries such as high-performance lithium batteries used in personal digital assistants, portable electronic devices, small household power storage devices, motorcycles powered by motors, electric vehicles, hybrid electric vehicles, etc. has increased. Yes.
As the applications for use expand, further improvements in safety and performance of secondary batteries are required.

  Inorganic solid electrolytes are generally nonflammable in nature and are safer materials than commonly used organic solvent electrolytes. Therefore, development of a lithium battery having high safety using the electrolyte is desired.

  Patent Document 1 discloses that when a solid electrolyte is applied to form a sheet, the solid electrolyte is suspended in a solvent and a binder is further added. At this time, the usable solvent for the sulfide-based solid electrolyte is limited to hydrocarbon solvents such as heptane and toluene. However, the hydrocarbon solvent is inactive in ionic conductivity and electronic conductivity, and it is not preferable to remain. When a battery is manufactured including the remaining hydrocarbon solvent, the battery performance is lowered.

In addition, until now, there is an example in which an electrolyte such as dimethyl carbonate is brought into contact with a Li ₂ S—SiS ₂ —Li ₃ PO ₄ electrolyte to examine its stability, but only changes in hue and the like were observed, No mention is made of the performance of the electrolyte or the effect of the battery (Non-Patent Document 1).

  As described above, when a sulfide-based electrolyte is used, usable solvents and binders are limited. In addition, it has been difficult to form a sheet using a highly polar polymer such as a polyether-based polymer or a polymer containing an electrolyte.

Patent Document 2 discloses an example in which a polyether binder and a lithium salt are mixed with an oxide solid electrolyte. However, ionic conductivity is not sufficient, and generally an oxide solid electrolyte has a particle interface. Since the resistance is large, there is a problem that the impedance increases when the battery is used.
JP 2005-353309 A JP 2007-220377 A New Energy and Industrial Technology Development Organization 2001 Results Report “Development of a New Inorganic Electrolyte for All Solid Lithium Batteries with Improved Stability”

  An object of the present invention is to provide a composition having good processability that can maintain a solid electrolyte while maintaining ionic conductivity and can disperse the solid electrolyte without lowering the ionic conductivity.

According to the present invention, the following composition, lithium battery and the like are provided.
1. A lithium ion conductive solid electrolyte comprising at least one element selected from phosphorus, silicon, germanium, and boron, lithium and sulfur;
1 or more types of compounds chosen from the carbonate compound represented by following formula (1), the ether compound represented by following formula (2), and the nitrile compound represented by following formula (3). A featured composition.
R ₁ —O—C (═O) —O—R ₂ (1)
(In Formula (1), R ₁ and R ₂ are each a group having 2 or more carbon atoms.)
R ₃ —O—R ₄ —O—R ₅ (2)
(In the formula _{(2), R 3, R} 5 are each the number 2 or more groups carbons, _{R 4} is one or more groups carbon atoms.)
R ₆ -CN (3)
(In Formula (3), R ₆ is a group having 2 or more carbon atoms.)
2. 2. The composition according to 1, further comprising a polymer compound.
3. The composition according to 1 or 2, further comprising a lithium electrolyte salt.
The solid electrolyte sheet manufactured using the composition as described in any one of 4.1-3.
A lithium battery using the solid electrolyte sheet described in 5.4.
An apparatus comprising the lithium battery according to 6.5.

  ADVANTAGE OF THE INVENTION According to this invention, a solid electrolyte is hold | maintained, maintaining ionic conductivity, and a composition with favorable workability can be provided.

The composition of the present invention includes a lithium ion conductive solid electrolyte and one or more compounds selected from a carbonate ester compound, an ether compound, and a nitrile compound (hereinafter also referred to as a carbonate ester compound). A carbonate ester compound or the like is used as a solvent. The composition of the present invention is a slurry or solution in which a solid electrolyte is dispersed or dissolved in a carbonate compound or the like.
Here, the composition of the present invention includes a solid electrolyte slurry (or a solid electrolyte solution) in which a solid electrolyte is dispersed or dissolved in a carbonate compound or the like, and a solid electrolyte and a positive electrode active material are dispersed or dissolved in a carbonate compound or the like. And a negative electrode mixture slurry or a negative electrode mixture solution obtained by dispersing or dissolving a solid electrolyte and a negative electrode active material in a carbonate compound or the like.

The lithium ion conductive solid electrolyte is composed of at least one element selected from phosphorus, silicon, germanium, and boron, and lithium and sulfur.
The lithium ion conductive solid electrolyte is produced by reacting lithium sulfide with phosphorus sulfide, germanium sulfide, silicon sulfide, and boron sulfide.

Lithium sulfide can be synthesized, for example, by the method described in Japanese Patent No. 3528866. Further, those purified by the method described in WO2005 / 040039 and having a purity of 99% or more are preferred.
The lithium sulfide preferably has an average particle size of 10 μm or less by a treatment such as pulverization in advance. More preferably, it is 5 μm or less. A small average particle size is advantageous in terms of reaction time and conductivity of the obtained solid electrolyte.

  Lithium sulfide can be reacted with phosphorus sulfide, germanium sulfide, silicon sulfide, and boron sulfide, with phosphorus sulfide being preferred. Among phosphorus sulfides, diphosphorus pentasulfide is particularly preferable.

  The proportion of lithium sulfide used as a raw material is 30 to 95 mol%, preferably 40 to 85 mol% of the total of one or more compounds selected from lithium sulfide and phosphorus sulfide, germanium sulfide, silicon sulfide and boron sulfide. Preferably it is 50-75 mol%.

  The solid electrolyte is synthesized using these raw materials by methods such as mechanical milling (Japanese Patent Laid-Open No. 2005-228570) and reaction in a solvent (Japanese Patent Laid-Open No. 2007-265523).

The carbonate compound is represented by the following formula (1).
R ₁ —O—C (═O) —O—R ₂ (1)
In formula (1), R ₁ and R ₂ are each a group having 2 or more carbon atoms.
Preferably, R ₁ and R ₂ are each an alkyl group, an alkenyl group, an alkynyl group, or a carbon number of 6 or more (more preferably) having 2 or more carbon atoms (more preferably 2 to 6 carbon atoms, particularly preferably 2 to 4 carbon atoms). An aryl group having 6 to 10 carbon atoms. Alkyl groups include straight chain alkyl, branched alkyl, and cyclic alkyl groups.
Specific examples include ethyl methyl carbonate, diethyl carbonate, dipropyl carbonate, dibutyl carbonate, and diphenyl carbonate.

The ether compound is represented by the following formula (2).
R ₃ —O—R ₄ —O—R ₅ (2)
In formula (2), R ₃ and R ₅ are each a group having 2 or more carbon atoms. R ₄ is a group having 1 or more carbon atoms.
Preferably, R ₃ and R ₅ are each an alkyl group, alkenyl group, alkynyl group or 6 or more carbon atoms (more preferably 2 or more carbon atoms, more preferably 2 to 4 carbon atoms, more preferably 2 to 4 carbon atoms). An aryl group having 6 to 10 carbon atoms, particularly preferably 2 to 4 carbon atoms.
R ₄ is preferably an alkylene group having 1 or more carbon atoms (more preferably 1 to 6 carbon atoms, particularly preferably 1 to 4 carbon atoms) or an arylene group having 6 or more carbon atoms (more preferably 6 to 10 carbon atoms). is there.
Specific examples include diethoxyethane, diethoxypropane, diethoxybutane, diethoxypropane and the like.

Nitrile compound is represented by the following formula (3).
R ₆ -CN (3)
In Formula (3), R ₆ is a group having 2 or more carbon atoms.
Preferably R ₆ is an alkyl group having 2 or more carbon atoms (more preferably 2 to 6 carbon atoms, particularly preferably 2 to 4 carbon atoms), an alkenyl group, an alkynyl group or having 6 or more carbon atoms (more preferably 6 to carbon atoms 10) an aryl group.
Specific examples include propionitrile and butyronitrile.

  The carbonate compound and the like are preferably dehydrated in advance. Specifically, the water content is preferably 100 ppm or less, more preferably 30 ppm or less.

  The carbonate ester compounds and the like may be used alone or in a mixture.

  If necessary, other solvents such as hydrocarbons such as hexane, heptane, decane, toluene and xylene, halogenated hydrocarbons such as dichloromethane and chlorobenzene, and the like can be added.

The composition of the present invention may further contain a polymer compound.
Here, the polymer compound is used as a binder for joining solid electrolyte particles together.
Although there is no restriction | limiting in particular as a high molecular compound, For example, polyether, polyolefin, (meth) acrylic resin, styrene butadiene rubber, silicone, an ethylene oxide propylene oxide copolymer, a polyethylene oxide resin etc. are mentioned. Preferable examples include those that can obtain ionic conductivity when combined with a lithium electrolyte salt such as polyether.

The composition of the present invention may further contain a lithium electrolyte salt. By including the lithium electrolyte salt, ionic conductivity can be improved.
Although there is no restriction | limiting in particular as lithium electrolyte salt, A well-known thing can be used.
Specifically, lithium hexafluorophosphate, lithium tetrafluoroborate, lithium perchlorate, lithium bis (trifluoromethanesulfonyl) imide, lithium bis (pentafluoroethanesulfonyl) imide, lithium trifluoromethanesulfonate, etc. Can be mentioned.

  The composition of this invention can contain a thickener etc. in the range which does not impair the effect of this invention.

The composition of the present invention is produced by mixing the above components.
Specifically, a solid electrolyte and a carbonate compound or the like (solvent) are mixed to produce a slurry or solution containing the solid electrolyte.
Here, it is preferable that the electrolyte does not swell due to absorption of a large amount of solvent. Usually, the electrolyte is 0.001 to 1 Kg / L-solvent, preferably 0.005 to 0.5 Kg / L-solvent, and more preferably 0.01 to 0.3 Kg / L-solvent.

In addition, a polymer compound and a lithium electrolyte salt can be appropriately added.
The addition amount of the polymer compound is preferably 0.1 to 10% by weight with respect to the solid electrolyte. The concentration with respect to the solvent is not particularly limited, but is usually about 0.1 to 10% by weight, preferably about 0.5 to 3% by weight, and more preferably about 0.7 to 2% by weight.
The addition amount of the lithium electrolyte salt is preferably 0.01 to 10% by weight with respect to the solid electrolyte.

The composition of the present invention can be used for a solid electrolyte layer or an electrode of a solid secondary battery such as a lithium battery.
FIG. 1 is a schematic cross-sectional view showing the structure of a solid secondary battery.
In the all solid state secondary battery 1, the solid electrolyte layer 20 is sandwiched between a pair of electrodes composed of a positive electrode 10 and a negative electrode 30, and current collectors 40 and 42 are provided on the positive electrode 10 and the negative electrode 30, respectively.
The composition of the present invention can be used for the solid electrolyte layer 20.
The positive electrode mixture slurry (or the positive electrode mixture solution) can be applied to the solid electrolyte layer 20 (or the positive electrode current collector) and then dried to form the positive electrode 10. Similarly, the negative electrode mixture 30 (or the negative electrode mixture solution) can be applied to the solid electrolyte layer 20 (or the negative electrode current collector) and then dried to form the negative electrode 30.
The above polymer compound, lithium electrolyte salt and the like can be appropriately added.
There is no particular restriction on the order of input. The temperature is preferably below the boiling point of the solvent and above the freezing point. A normal stirrer can be used for mixing.

As the positive electrode active material, a metal oxide capable of inserting and desorbing lithium ions and those known as positive electrode active materials in the battery field can be used.
For example, in the sulfide system, titanium sulfide (TiS ₂ ), molybdenum sulfide (MoS ₂ ), iron sulfide (FeS, FeS ₂ ), copper sulfide (CuS), nickel sulfide (Ni ₃ S ₂ ), etc. can be used. TiS ₂ is preferred. These substances can be used alone or in combination of two or more.
In the oxide system, bismuth oxide (Bi ₂ O ₃ ), bismuth lead acid (Bi ₂ Pb ₂ O ₅ ), copper oxide (CuO), vanadium oxide (V ₆ O ₁₃ ), lithium cobalt oxide (LiCoO ₂ ) , Lithium nickelate (LiNiO ₂ ), lithium manganate (LiMn ₂ O ₄ ), olivine-type lithium iron phosphate (LiFePO ₄ ), nickel-manganese oxide (LiNi _0.5 Mn _0.5 O ₂ ), Nickel-aluminum-cobalt oxide (LiNi _0.08 Co _0.15 Al _0.15 O ₂ ), nickel-manganese-cobalt oxide (LiNi _0.33 Co _0.33 Mn _0.33 O ₂ ), etc. LiCoO ₂ and LiNi _0.08 Co _0.15 Al _0.15 O ₂ are particularly suitable. These substances can be used alone or in combination of two or more.
It is also possible to use a mixture of the above sulfides and oxides. In addition to the above, niobium selenide (NbSe ₃ ) can also be used.

As the negative electrode active material, a material capable of inserting and desorbing lithium ions, and a material known as a negative electrode active material in the battery field can be used.
For example, carbon materials, specifically artificial graphite, graphite carbon fiber, resin-fired carbon, pyrolytic vapor-grown carbon, coke, mesocarbon microbeads (MCMB), furfuryl alcohol resin-fired carbon, polyacene, pitch-based carbon Examples thereof include fibers, vapor-grown carbon fibers, natural graphite and non-graphitizable carbon, and artificial graphite is particularly preferable.
An alloy combined with a metal itself such as metallic lithium, metallic indium, metallic aluminum, metallic silicon, metallic tin, or another element or compound can be used as the negative electrode active material.
These negative electrode active materials can be used individually by 1 type or in combination of 2 or more types.

The method for forming the solid electrolyte layer or the electrode is not particularly limited as long as it can be formed into a sheet shape. For example, a forming method such as press molding or roll press molding, a sheet forming method by a coating method such as doctor blade or screen printing, and the like can be mentioned.
Of these, it is preferable to form a sheet by coating. The composition of the present invention is mainly composed of the solid electrolyte and the organic solvent. If necessary, a binder such as a resin (the polymer compound), a thickener, and the like may be added. For example, the composition can be applied and dried using a doctor blade or the like, formed into a sheet, and then the solid electrolyte formed into a sheet by pressing or roll pressing can be consolidated. A roll press is particularly preferable. The pressing pressure is preferably about 30 MPa to 1000 MPa.
The temperature at that time may be any as long as the material does not decompose or deteriorate, and is usually 300 ° C. or lower. When making an electrode or a solid electrolyte sheet, a solvent may be intentionally included in the solid electrolyte and left as it is.

Production Example 1
<Manufacture of solid electrolyte>
A solid electrolyte containing lithium, sulfur and phosphorus was synthesized according to the method described in JP-A-2005-228570. Specifically, it was synthesized as follows.
A 45 mL alumina container containing about 1 g of a mixture of Li ₂ S and P ₂ S ₅ (manufactured by Aldrich) (molar ratio of Li ₂ S to P ₂ S ₅ ; 68:32) and 10 alumina balls having a diameter of 10 mm And then subjected to mechanical milling for 20 hours at room temperature (25 ° C.) in nitrogen at room temperature (25 ° C.) with a planetary ball mill (manufactured by Fritsch: Model No. P-7), and sulfurized as a white yellow powder A physical glass was obtained.
The powder was heat-treated at 300 ° C. for 2 hours under a nitrogen stream to obtain a lithium ion conductive material having an average particle size of 10 μm.
The obtained lithium ion conductive material was used as a solid electrolyte in the following Examples and Comparative Examples.

Example 1
<Production of composition>
Under a nitrogen stream, 15 mL of diethyl carbonate (moisture 30 ppm or less manufactured by Kishida Chemical Co., Ltd.) was added to 5 g of the solid electrolyte, and stirred for 1 hour to prepare a composition.
The solvent was vacuum-dried at room temperature, and further heat-dried at 150 ° C. for 1 hour. The obtained dry electrolyte (hereinafter referred to as “dry solid electrolyte”) had an ionic conductivity of 1.2 × 10 ⁻³ S / cm.
In Examples and Comparative Examples, ionic conductivity was measured by an AC impedance method.

Example 2
<Production of composition>
A composition was prepared in the same manner as in Example 1 except that diethoxyethane (water content of 50 ppm or less manufactured by Kishida Chemical Co., Ltd.) was used instead of diethyl carbonate. The ionic conductivity of the dried solid electrolyte obtained by drying the composition was 1.1 × 10 ⁻³ S / cm.

Example 3
<Production of composition>
A composition was prepared in the same manner as in Example 1 except that propionitrile (water content of 30 ppm or less manufactured by Kishida Chemical Co., Ltd.) was used instead of diethyl carbonate. Ion conductivity of the resulting dry solid electrolyte by drying the composition was 1.1 × 10 -3 ^{S /} cm.

Comparative Example 1
<Production of composition>
A composition was prepared in the same manner as in Example 1 except that dimethyl carbonate (manufactured by Kishida Chemical Co., Ltd., water content of 30 ppm or less) was used instead of diethyl carbonate. The ionic conductivity of the dried solid electrolyte obtained by drying the composition was 4.2 × 10 ⁻⁶ S / cm.

Comparative Example 2
<Production of composition>
A composition was prepared in the same manner as in Example 2, except that dimethoxyethane (water content of 30 ppm or less manufactured by Kishida Chemical Co., Ltd.) was used instead of diethoxyethane. The ionic conductivity of the dried solid electrolyte obtained by drying the composition was 3.0 × 10 ⁻⁷ S / cm.

Comparative Example 3
<Production of composition>
A composition was prepared in the same manner as in Example 3 except that acetonitrile (water content of 30 ppm or less manufactured by Kishida Chemical Co., Ltd.) was used instead of propionitrile. The ionic conductivity of the dried solid electrolyte obtained by drying the composition was 1.6 × 10 ⁻⁷ S / cm.

Example 4
<Manufacture of solid electrolyte sheet>
Under a nitrogen stream, 15 mL of diethyl carbonate, 0.26 g of ethylene oxide-propylene oxide copolymer and 0.065 g of lithium salt (lithium trifluoromethanesulfonate) were added and stirred at room temperature. The copolymer and lithium salt were dissolved in a solvent. Further, 5 g of solid electrolyte was added and stirred for 1 hour. The slurry was applied on an aluminum sheet using a bar coater, and then the solvent was dried at room temperature and further dried by heating at 150 ° C. for 1 hour. A flexible sheet containing the electrolyte was obtained. The ionic conductivity of the obtained solid electrolyte sheet was 8.0 × 10 ⁻⁴ S / cm.

Example 5
<Manufacture of solid electrolyte sheet>
A sheet was prepared in the same manner as in Example 4 except that diethoxyethane was used instead of diethyl carbonate.
A flexible sheet containing the electrolyte was obtained. The ionic conductivity of the obtained solid electrolyte sheet was 7.3 × 10 ⁻⁴ S / cm.

Example 6
<Manufacture of solid electrolyte sheet>
A sheet was produced in the same manner as in Example 4 except that propion carbonate was used instead of diethyl carbonate.
The ionic conductivity of the obtained solid electrolyte sheet was 5.0 × 10 ⁻⁴ S / cm.

Example 7
<Manufacture of solid electrolyte sheet>
To 15 ml of diethyl carbonate, 0.065 g of lithium salt (lithium trifluoromethanesulfonate) (manufactured by Kishida Chemical Co., Ltd.) was added and dissolved. Further, 0.26 g of polyethylene oxide resin (Meisei Chemical Co., Ltd., Alcox E60) was added. A clear viscous solution was obtained. To this, 5 g of a solid electrolyte was added to obtain a composition. The slurry was applied on an aluminum sheet using a bar coater, and then the solvent was dried at room temperature and further dried by heating at 150 ° C. for 1 hour. A flexible sheet containing the electrolyte was obtained. The ionic conductivity of the obtained solid electrolyte sheet was 3.3 × 10 ⁻⁴ S / cm.

Comparative Example 4
<Manufacture of solid electrolyte sheet>
Under a nitrogen stream, 0.26 g of ethylene oxide-propylene oxide copolymer and 0.065 g of lithium salt (lithium trifluoromethanesulfonate) were added to 15 ml of toluene (Wako Pure Chemical Industries, Ltd., water content of 30 ppm or less) and stirred at room temperature. The resin did not dissolve and a gel-like precipitate was formed. After adding 5 g of solid electrolyte to this and making it into a slurry, it was applied onto an aluminum sheet using a bar coater. However, the electrolyte and the gel-like substance were separated and could not be applied uniformly.

Comparative Example 5
<Manufacture of solid electrolyte sheet>
Under nitrogen flow, 0.26 g of polyethylene oxide resin (Meisei Chemical Co., Ltd. Alcox E60) and 0.065 g of lithium salt (lithium trifluoromethanesulfonate) (manufactured by Kishida Chemical Co., Ltd.) in 15 ml of toluene (Wako Pure Chemical Industries moisture 30 ppm or less) Was added. A gel-like precipitate was formed. After adding 5 g of solid electrolyte to this and making it into a slurry, it was applied onto an aluminum sheet using a bar coater. However, the electrolyte and the gel-like substance were separated and could not be applied uniformly.

Example 8
<Manufacture of batteries>
An electrolyte layer was prepared by molding 0.2 g of the dry solid electrolyte prepared in Example 1 in a mold. A positive electrode active material LNCAO (manufactured by Toda Kogyo Co., Ltd.) and 0.1 g of the dry solid electrolyte mixture produced in Example 1 (positive electrode active material: electrolyte = 7: 3) were added and molded again, and the positive electrode, electrolyte layer A layered pellet having An In foil was placed as a negative electrode so as to be in contact with the electrolyte layer on the opposite side of the positive electrode, and this was accommodated in a battery container, sealed, and pressed with a 20 kgf / cm ² spring to produce a battery. The resulting initial charge-discharge performance of the battery, 155 mAh / g at charge 0.2 mA / cm ^2, was 110 mAh / g at a discharge 0.2 mA / cm ^2.

Example 9
<Manufacture of batteries>
A battery was produced in the same manner as in Example 8 using the dry solid electrolyte produced in Example 2. The initial charge / discharge performance of the obtained battery was 145 mAh / g at a charge of 0.2 mA / cm ² and 105 mAh / g at a discharge of 0.2 mA / cm ² .

Comparative Example 6
<Manufacture of batteries>
A battery was fabricated in the same manner as in Example 8 using the solid electrolyte (lithium ion conductive material) obtained in Production Example 1 which was not treated by adding a solvent and drying. The resulting initial charge-discharge performance of the battery, 140 mAh / g at charge 0.2 mA / cm ^2, was 100 mAh / g at a discharge 0.2 mA / cm ^2.

  The composition of the present invention can be used for a solid electrolyte layer and an electrode of a solid secondary battery. Such a solid secondary battery can be used as a battery for a portable information terminal, a portable electronic device, a small electric power storage device for home use, a motorcycle using a motor as a power source, an electric vehicle, a hybrid electric vehicle, or the like.

It is a schematic sectional drawing which shows the structure of an all-solid-state secondary battery.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 All-solid-state secondary battery 10 Positive electrode 20 Solid electrolyte layer 30 Negative electrode 40,42 Current collector

Claims (6)

A lithium ion conductive solid electrolyte comprising at least one element selected from phosphorus, silicon, germanium, and boron, lithium and sulfur;
1 or more types of compounds chosen from the carbonate compound represented by following formula (1), the ether compound represented by following formula (2), and the nitrile compound represented by following formula (3). A featured composition.
R ₁ —O—C (═O) —O—R ₂ (1)
(In Formula (1), R ₁ and R ₂ are each a group having 2 or more carbon atoms.)
_{R 3 -O-R 4 -O-} R 5 (2)
(In Formula (2), R ₃ and R ₅ are each a group having 2 or more carbon atoms, and R ₄ is a group having 1 or more carbon atoms.)
R ₆ -CN (3)
(In Formula (3), R ₆ is a group having 2 or more carbon atoms.)   The composition according to claim 1, further comprising a polymer compound.   The composition according to claim 1 or 2, further comprising a lithium electrolyte salt.   The solid electrolyte sheet manufactured using the composition as described in any one of Claims 1-3.   A lithium battery using the solid electrolyte sheet according to claim 4.   An apparatus comprising the lithium battery according to claim 5.

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