JPWO2019151376A1 - 固体電池および固体電池の製造方法 - Google Patents
固体電池および固体電池の製造方法 Download PDFInfo
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- 238000004519 manufacturing process Methods 0.000 title claims abstract description 26
- 239000007784 solid electrolyte Substances 0.000 claims abstract description 112
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 102
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims abstract description 100
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 72
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 71
- 229910001148 Al-Li alloy Inorganic materials 0.000 claims abstract description 43
- JFBZPFYRPYOZCQ-UHFFFAOYSA-N [Li].[Al] Chemical compound [Li].[Al] JFBZPFYRPYOZCQ-UHFFFAOYSA-N 0.000 claims abstract description 43
- 239000001989 lithium alloy Substances 0.000 claims abstract description 43
- 238000000034 method Methods 0.000 claims abstract description 33
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- 238000007599 discharging Methods 0.000 abstract description 42
- 230000007423 decrease Effects 0.000 abstract description 19
- 239000007787 solid Substances 0.000 abstract description 9
- 230000008569 process Effects 0.000 abstract description 8
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 25
- 239000000203 mixture Substances 0.000 description 21
- 230000000052 comparative effect Effects 0.000 description 16
- 239000012071 phase Substances 0.000 description 14
- 229910018091 Li 2 S Inorganic materials 0.000 description 12
- 229910010199 LiAl Inorganic materials 0.000 description 9
- 239000010408 film Substances 0.000 description 7
- 229910001416 lithium ion Inorganic materials 0.000 description 7
- 239000002994 raw material Substances 0.000 description 7
- 238000013329 compounding Methods 0.000 description 6
- 239000007774 positive electrode material Substances 0.000 description 6
- 239000000843 powder Substances 0.000 description 6
- 229910018130 Li 2 S-P 2 S 5 Inorganic materials 0.000 description 5
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 5
- 229910020346 SiS 2 Inorganic materials 0.000 description 5
- 238000005304 joining Methods 0.000 description 5
- 239000007773 negative electrode material Substances 0.000 description 5
- 239000002203 sulfidic glass Substances 0.000 description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 4
- 230000014759 maintenance of location Effects 0.000 description 4
- 238000000465 moulding Methods 0.000 description 4
- 239000010409 thin film Substances 0.000 description 4
- 229910018133 Li 2 S-SiS 2 Inorganic materials 0.000 description 3
- 238000002441 X-ray diffraction Methods 0.000 description 3
- 229910045601 alloy Inorganic materials 0.000 description 3
- 239000000956 alloy Substances 0.000 description 3
- 238000005275 alloying Methods 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 229910052732 germanium Inorganic materials 0.000 description 3
- 239000003960 organic solvent Substances 0.000 description 3
- 229910052698 phosphorus Inorganic materials 0.000 description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 229910018111 Li 2 S-B 2 S 3 Inorganic materials 0.000 description 2
- 229910018127 Li 2 S-GeS 2 Inorganic materials 0.000 description 2
- 229910000733 Li alloy Inorganic materials 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- -1 and the like Chemical compound 0.000 description 2
- 229910052796 boron Inorganic materials 0.000 description 2
- 229910052794 bromium Inorganic materials 0.000 description 2
- 229910052801 chlorine Inorganic materials 0.000 description 2
- 239000004020 conductor Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 239000003792 electrolyte Substances 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 229910052733 gallium Inorganic materials 0.000 description 2
- 229910052736 halogen Inorganic materials 0.000 description 2
- 150000002367 halogens Chemical class 0.000 description 2
- 229910052740 iodine Inorganic materials 0.000 description 2
- 229910052742 iron Inorganic materials 0.000 description 2
- HSZCZNFXUDYRKD-UHFFFAOYSA-M lithium iodide Inorganic materials [Li+].[I-] HSZCZNFXUDYRKD-UHFFFAOYSA-M 0.000 description 2
- WPBNNNQJVZRUHP-UHFFFAOYSA-L manganese(2+);methyl n-[[2-(methoxycarbonylcarbamothioylamino)phenyl]carbamothioyl]carbamate;n-[2-(sulfidocarbothioylamino)ethyl]carbamodithioate Chemical compound [Mn+2].[S-]C(=S)NCCNC([S-])=S.COC(=O)NC(=S)NC1=CC=CC=C1NC(=S)NC(=O)OC WPBNNNQJVZRUHP-UHFFFAOYSA-L 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 238000003825 pressing Methods 0.000 description 2
- 238000001878 scanning electron micrograph Methods 0.000 description 2
- 229910052710 silicon Inorganic materials 0.000 description 2
- 238000001228 spectrum Methods 0.000 description 2
- 229910001220 stainless steel Inorganic materials 0.000 description 2
- 239000010935 stainless steel Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000010936 titanium Substances 0.000 description 2
- 229910052719 titanium Inorganic materials 0.000 description 2
- 229910052720 vanadium Inorganic materials 0.000 description 2
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 description 2
- 229910052725 zinc Inorganic materials 0.000 description 2
- 239000011701 zinc Substances 0.000 description 2
- 229910005839 GeS 2 Inorganic materials 0.000 description 1
- 229910018068 Li 2 O Inorganic materials 0.000 description 1
- 229910009324 Li2S-SiS2-Li3PO4 Inorganic materials 0.000 description 1
- 229910009320 Li2S-SiS2-LiBr Inorganic materials 0.000 description 1
- 229910009316 Li2S-SiS2-LiCl Inorganic materials 0.000 description 1
- 229910009318 Li2S-SiS2-LiI Inorganic materials 0.000 description 1
- 229910009328 Li2S-SiS2—Li3PO4 Inorganic materials 0.000 description 1
- 229910007281 Li2S—SiS2—B2S3LiI Inorganic materials 0.000 description 1
- 229910007295 Li2S—SiS2—Li3PO4 Inorganic materials 0.000 description 1
- 229910007291 Li2S—SiS2—LiBr Inorganic materials 0.000 description 1
- 229910007288 Li2S—SiS2—LiCl Inorganic materials 0.000 description 1
- 229910007289 Li2S—SiS2—LiI Inorganic materials 0.000 description 1
- 229910007306 Li2S—SiS2—P2S5LiI Inorganic materials 0.000 description 1
- 229910013733 LiCo Inorganic materials 0.000 description 1
- 229910012735 LiCo1/3Ni1/3Mn1/3O2 Inorganic materials 0.000 description 1
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 1
- 229910011281 LiCoPO 4 Inorganic materials 0.000 description 1
- 229910010707 LiFePO 4 Inorganic materials 0.000 description 1
- 229910015643 LiMn 2 O 4 Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 239000002178 crystalline material Substances 0.000 description 1
- 238000002425 crystallisation Methods 0.000 description 1
- 230000008025 crystallization Effects 0.000 description 1
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- 238000000151 deposition Methods 0.000 description 1
- 238000007607 die coating method Methods 0.000 description 1
- 238000003618 dip coating Methods 0.000 description 1
- 238000004070 electrodeposition Methods 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 229910052737 gold Inorganic materials 0.000 description 1
- 239000010931 gold Substances 0.000 description 1
- 229910021385 hard carbon Inorganic materials 0.000 description 1
- 230000000887 hydrating effect Effects 0.000 description 1
- 230000036571 hydration Effects 0.000 description 1
- 238000006703 hydration reaction Methods 0.000 description 1
- 229910052738 indium Inorganic materials 0.000 description 1
- 239000010416 ion conductor Substances 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 150000004715 keto acids Chemical class 0.000 description 1
- 238000010030 laminating Methods 0.000 description 1
- 239000011572 manganese Substances 0.000 description 1
- 238000003701 mechanical milling Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 238000010587 phase diagram Methods 0.000 description 1
- 239000011574 phosphorus Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 238000004080 punching Methods 0.000 description 1
- 230000000452 restraining effect Effects 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 238000007650 screen-printing Methods 0.000 description 1
- 238000010532 solid phase synthesis reaction Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
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- 239000011029 spinel Substances 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 150000004763 sulfides Chemical class 0.000 description 1
- 229910052717 sulfur Inorganic materials 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
- 238000003826 uniaxial pressing Methods 0.000 description 1
Classifications
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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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/381—Alkaline or alkaline earth metals elements
- H01M4/382—Lithium
-
- 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
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- 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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- H01M10/058—Construction or manufacture
- H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
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- H—ELECTRICITY
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- H01M4/00—Electrodes
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- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/134—Electrodes based on metals, Si or alloys
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Abstract
Description
以下、本発明の固体電池の一実施形態について、図面を参照しながら詳細に説明する。図1は、本発明の一実施形態に係る固体電池の断面を示す説明図である。図1に示すように固体電池1は、電池本体10と、負極集電体50と、正極集電体60とを備える。なお、本明細書において、固体電池とは電池を全固体化したものをいう。
次に、本発明の一実施形態に係る固体電池1の製造方法について、図面を参照しながら説明する。図8は、本発明の一実施形態に係る固体電池の製造方法を示す説明図である。図9は、本発明の一実施形態に係る固体電池の製造方法における、切断工程の一例を示す説明図である。図8に示すように、固体電池1の製造方法は、固体電解質材塗布工程と、圧接接合工程と、切断工程とを含む。
本実施形態に係る固体電解質材塗布工程は、アルミニウム層31を形成するためのアルミニウム板上に固体電解質材を塗布して、固体電解質層40を形成する工程である。固体電解質材を塗布する方法としては、例えば、ダイコート法、スプレーコート法、転写シート法、ディップコート法、スクリーン印刷法等を挙げることができる。
本実施形態に係る圧接接合工程は、アルミニウム層31を形成するためのアルミニウム板の固体電解質層40が形成された一面上に、正極電極層20を配置するとともに、アルミニウム板の固体電解質層40が形成されていない他面上に、リチウム層32を形成するためのリチウム板を配置して得られる積層体を圧接接合することにより、固体電池1を得る工程である。
切断工程は、圧接接合された電池本体を、所定長さに切断する工程である。図9に示すように、本実施形態においては、切断工程は、圧接接合された電池本体10を、圧縮しながら所定長さに切断する工程である。
厚みが100μmのアルミニウム箔と、厚みが100μmのリチウム箔とを重ね合わせて、実施例1の負極電極層とした。
アルミニウム−リチウム合金粉末をプレス成型して比較例1の負極電極層とした。
負極電極層における、リチウムとアルミニウムとの合計を100mol%とした場合に、リチウムがそれぞれ38mol%(実施例2)、44mol%(実施例3)、50mol%(実施例4)60mol%(実施例5)、80mol%(実施例6)となるようにアルミニウム板と、リチウム板とを重ね合わせて、実施例2〜実施例6の負極電極層とした。
予めアルミニウム板の上に固体電解質層を塗工した電極に対し、正極層を塗工した電極を重ね、一軸プレスにて4.5ton/cm2の加圧力にて加圧成形した。その後、リチウム板を負極電極層の下部に配置し、1ton/cm2の加圧力にて加圧成形し、固体電池を作製した。負極電極層としては、厚みが100μmのアルミニウム板と、厚みが100μmのリチウム板とを用いた。
ハードカーボン(負極活物質)と固体電解質とを55:45wt%の比率で混合した合材電極を、一軸プレスにて3ton/cm2の加圧力にて成形した。成形後の負極電極層に固体電解質層を塗工した。その後、正極層を塗工した電極を重ね、一軸プレスにて4.5ton/cm2の加圧力にて加圧成形し、固体電池を作製した。
20 正極電極層
30 負極電極層
31 アルミニウム層
32 リチウム層
33 アルミニウム−リチウム合金層
40 固体電解質層
Claims (7)
- 正極電極層と、負極電極層と、前記正極電極層と前記負極電極層との間に配置される固体電解質層と、を備え、
前記負極電極層は、前記固体電解質層と接するアルミニウム層と、リチウム層と、前記アルミニウム層と前記リチウム層との間に配置されるアルミニウム−リチウム合金層と、を備える固体電池。 - 前記負極電極層の膜厚は、10〜400μmである、請求項1に固体電池。
- 前記負極電極層におけるリチウムと、アルミニウムとのモル比率は、Li:Al=30:70〜80:20である、請求項1または2に固体電池。
- 前記固体電解質層は、硫化物系固体電解質材料である、請求項1〜3のいずれかに固体電池。
- 正極電極層と、アルミニウム層およびリチウム層を備える負極電極層と、前記正極電極層と前記負極電極層との間に配置される固体電解質層と、を備える固体電池の製造方法であって、
前記アルミニウム層を形成するためのアルミニウム板上に固体電解質材を塗布して、前記固体電解質層を形成する、固体電解質材塗布工程と、
前記アルミニウム板の前記固体電解質層が形成された一面上に、前記正極電極層を配置するとともに、前記アルミニウム板の前記固体電解質層が形成されていない他面上に、前記リチウム層を形成するためのリチウム板を配置して得られる積層体を、圧接接合することにより固体電池を得る、圧接接合工程と、
を備える固体電池の製造方法。 - 前記圧接接合された固体電池を、圧縮しながら所定長さに切断する、切断工程を更に備える請求項5に記載の固体電池の製造方法。
- 前記圧接接合工程は、ロールプレス法によって行われる請求項5または6に記載の固体電池の製造方法。
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