JP7417925B2 - 固体電解質材料、および、電池 - Google Patents
固体電解質材料、および、電池 Download PDFInfo
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- JP7417925B2 JP7417925B2 JP2019563935A JP2019563935A JP7417925B2 JP 7417925 B2 JP7417925 B2 JP 7417925B2 JP 2019563935 A JP2019563935 A JP 2019563935A JP 2019563935 A JP2019563935 A JP 2019563935A JP 7417925 B2 JP7417925 B2 JP 7417925B2
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- solid electrolyte
- electrolyte material
- positive electrode
- negative electrode
- battery
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Classifications
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0562—Solid materials
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
- C01F17/00—Compounds of rare earth metals
- C01F17/30—Compounds containing rare earth metals and at least one element other than a rare earth metal, oxygen or hydrogen, e.g. La4S3Br6
- C01F17/36—Compounds containing rare earth metals and at least one element other than a rare earth metal, oxygen or hydrogen, e.g. La4S3Br6 halogen being the only anion, e.g. NaYF4
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G15/00—Compounds of gallium, indium or thallium
- C01G15/006—Compounds containing, besides gallium, indium, or thallium, two or more other elements, with the exception of oxygen or hydrogen
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
- C01G29/00—Compounds of bismuth
- C01G29/006—Compounds containing, besides bismuth, two or more other elements, with the exception of oxygen or hydrogen
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- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
- H01B1/06—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
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- C—CHEMISTRY; METALLURGY
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- C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- C01P2004/00—Particle morphology
- C01P2004/60—Particles characterised by their size
- C01P2004/61—Micrometer sized, i.e. from 1-100 micrometer
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- H—ELECTRICITY
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- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
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Description
実施の形態1における固体電解質材料は、下記の組成式(1)により表される固体電解質材料である。
Li3-3δY1+δ-aMaCl6-x-yBrxIy ・・・式(1)
ここで、Mは、Al、Sc、Ga、Biからなる群より選択される1種または2種以上の元素である。
-1<δ<1、
0<a<2、
0<(1+δ-a)、
0≦x≦6、
0≦y≦6、
(x+y)≦6、
が満たされる。
実施の形態1における固体電解質材料は、例えば、下記の方法により、製造されうる。
以下、実施の形態2が説明される。上述の実施の形態1と重複する説明は、適宜、省略される。
[固体電解質材料の作製]
露点-60℃以下のアルゴン雰囲気で、原料粉LiClとYCl3とBiCl3とを、モル比でLiCl:YCl3:BiCl3=3:0.95:0.05となるように、秤量した。これらを乳鉢で粉砕して混合した。その後、遊星型ボールミルを用い、25時間、600rpmでミリング処理した。
図2は、イオン伝導度の評価方法を示す模式図である。
σ=(RSE×S/t)-1 ・・・・(2)
ここで、σはイオン伝導度、Sは電解質面積(図2中、枠型301の内径)、Rは上記のインピーダンス測定における固体電解質の抵抗値、tは電解質の厚み(図2中、複数の固体電解質粒子100の圧縮体の厚み)である。
アルゴングローブボックス内で、実施例1の固体電解質材料と、活物質であるLiCoO2(以下、LCOと表記する)を、70:30の体積比率で秤量した。これらをメノウ乳鉢で混合することで、合剤を作製した。
図4は、初期放電特性を示すグラフである。
以下、Li3-3δY1+δ-aMaCl6-x-yBrxIyの合成および評価方法について説明する。
実施例2~22においては、露点-90℃以下、酸素値5ppm以下のドライ・低酸素雰囲気で保たれるグローブボックス内で、原料粉を秤量した。
露点-90℃以下、酸素値5ppm以下のドライ・低酸素雰囲気で保たれるグローブボックス内で、上記の実施例1と同様の方法で、実施例2~22のそれぞれの伝導度測定セルを作製した。
露点-90℃以下、酸素値5ppm以下のドライ・低酸素雰囲気で保たれるグローブボックス内で、実施例2~22のそれぞれの固体電解質材料と、正極活物質であるLiCoO2を、30:70の体積比率で秤量した。これらをメノウ乳鉢で混合することで、実施例2~22のそれぞれの正極合剤を作製した。
上記の実施例1と同様の方法で、実施例2~22のそれぞれの二次電池の充放電試験を行った。
固体電解質の原料粉として、LiClとFeCl2とを用いて、LiCl:FeCl2=2:1のモル比で混合した。
実施例1~22は、比較例1と比較して、室温近傍において、1×10-5S/cm以上の高いイオン伝導性を示すことがわかる。
201 正極
202 電解質層
203 負極
204 正極活物質粒子
205 負極活物質粒子
300 加圧成形用ダイス
301 枠型
302 パンチ下部
303 パンチ上部
1000 電池
Claims (6)
- 組成式Li3-3δY1+δ-aMaCl6-x-yBrxIyで表され、
ここで、Mは、Al、Sc、Ga、及びBiからなる群より選択される少なくとも1種であり、
-1<δ<1、
0<a<2、
0<(1+δ-a)、
0≦x≦6、
0≦y≦6、
(x+y)≦6、
を満たす、
固体電解質材料。 - 0.025≦a≦0.99、
を満たす、
請求項1に記載の固体電解質材料。 - 0.035≦a≦0.1、
を満たす、
請求項2に記載の固体電解質材料。 - -0.5≦δ≦0.5、
を満たす、
請求項1から3のいずれかに記載の固体電解質材料。 - -0.3≦δ≦0.2、
を満たす、
請求項4に記載の固体電解質材料。 - 請求項1から5のいずれかに記載の固体電解質材料と、
正極と、
負極と、
前記正極と前記負極との間に配置された電解質層と、
を備え、
前記正極と前記負極と前記電解質層とのうちの少なくとも1つは、前記固体電解質材料を含む、
電池。
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US11784345B2 (en) | 2023-10-10 |
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