CN1338129A - 非水电解质电池 - Google Patents
非水电解质电池 Download PDFInfo
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- CN1338129A CN1338129A CN00803016A CN00803016A CN1338129A CN 1338129 A CN1338129 A CN 1338129A CN 00803016 A CN00803016 A CN 00803016A CN 00803016 A CN00803016 A CN 00803016A CN 1338129 A CN1338129 A CN 1338129A
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- nonaqueous electrolyte
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- 239000011255 nonaqueous electrolyte Substances 0.000 title claims abstract description 61
- 239000000654 additive Substances 0.000 claims abstract description 36
- 230000000996 additive effect Effects 0.000 claims abstract description 35
- 239000002904 solvent Substances 0.000 claims abstract description 26
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 14
- 239000000463 material Substances 0.000 claims abstract description 7
- 229910000733 Li alloy Inorganic materials 0.000 claims abstract description 5
- 239000001989 lithium alloy Substances 0.000 claims abstract description 5
- 229910052731 fluorine Inorganic materials 0.000 claims description 22
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims description 22
- 230000014509 gene expression Effects 0.000 claims description 20
- 125000000217 alkyl group Chemical group 0.000 claims description 13
- 150000001875 compounds Chemical class 0.000 claims description 12
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 10
- 229910052788 barium Inorganic materials 0.000 claims description 10
- 229910052791 calcium Inorganic materials 0.000 claims description 10
- 229910052749 magnesium Inorganic materials 0.000 claims description 10
- 229910052712 strontium Inorganic materials 0.000 claims description 10
- 229910052792 caesium Inorganic materials 0.000 claims description 9
- 229910052700 potassium Inorganic materials 0.000 claims description 9
- 229910052701 rubidium Inorganic materials 0.000 claims description 9
- 229910052708 sodium Inorganic materials 0.000 claims description 9
- 229910052794 bromium Inorganic materials 0.000 claims description 8
- 229910052799 carbon Inorganic materials 0.000 claims description 8
- 229910052801 chlorine Inorganic materials 0.000 claims description 8
- 229910052740 iodine Inorganic materials 0.000 claims description 8
- 229910003002 lithium salt Inorganic materials 0.000 claims description 6
- ZZXUZKXVROWEIF-UHFFFAOYSA-N 1,2-butylene carbonate Chemical compound CCC1COC(=O)O1 ZZXUZKXVROWEIF-UHFFFAOYSA-N 0.000 claims description 5
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- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 claims description 5
- 229910013870 LiPF 6 Inorganic materials 0.000 claims description 4
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- 229910013684 LiClO 4 Inorganic materials 0.000 claims description 3
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- 230000015572 biosynthetic process Effects 0.000 claims description 2
- 159000000002 lithium salts Chemical class 0.000 claims description 2
- XKJCHHZQLQNZHY-UHFFFAOYSA-N phthalimide Chemical compound C1=CC=C2C(=O)NC(=O)C2=C1 XKJCHHZQLQNZHY-UHFFFAOYSA-N 0.000 abstract description 10
- CIFFBTOJCKSRJY-UHFFFAOYSA-N 3α,4,7,7α-tetrahydro-1h-isoindole-1,3(2h)-dione Chemical compound C1C=CCC2C(=O)NC(=O)C21 CIFFBTOJCKSRJY-UHFFFAOYSA-N 0.000 abstract description 4
- 230000000694 effects Effects 0.000 abstract description 3
- PXZQEOJJUGGUIB-UHFFFAOYSA-N isoindolin-1-one Chemical compound C1=CC=C2C(=O)NCC2=C1 PXZQEOJJUGGUIB-UHFFFAOYSA-N 0.000 abstract 2
- SPAMRUYRVYMHPV-UHFFFAOYSA-N 3a,4,5,7a-tetrahydroisoindole-1,3-dione Chemical class C1=CCCC2C(=O)NC(=O)C21 SPAMRUYRVYMHPV-UHFFFAOYSA-N 0.000 abstract 1
- 230000007774 longterm Effects 0.000 abstract 1
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- -1 poly(ethylene oxide) Polymers 0.000 description 10
- 239000011737 fluorine Substances 0.000 description 9
- JUJWROOIHBZHMG-UHFFFAOYSA-N Pyridine Chemical compound C1=CC=NC=C1 JUJWROOIHBZHMG-UHFFFAOYSA-N 0.000 description 8
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- 125000001153 fluoro group Chemical group F* 0.000 description 5
- UTVYDZFWHRCJCA-UHFFFAOYSA-N 7a-ethyl-3ah-isoindole-1,3-dione Chemical compound C1=CC=CC2C(=O)NC(=O)C21CC UTVYDZFWHRCJCA-UHFFFAOYSA-N 0.000 description 4
- OYLKIWHHTFETCW-UHFFFAOYSA-N isoindole-1,3-dione;pyridine Chemical compound C1=CC=NC=C1.C1=CC=C2C(=O)NC(=O)C2=C1 OYLKIWHHTFETCW-UHFFFAOYSA-N 0.000 description 4
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 4
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 3
- 206010013786 Dry skin Diseases 0.000 description 3
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 3
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- 229910044991 metal oxide Inorganic materials 0.000 description 3
- 150000004706 metal oxides Chemical class 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
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- SPEUIVXLLWOEMJ-UHFFFAOYSA-N 1,1-dimethoxyethane Chemical compound COC(C)OC SPEUIVXLLWOEMJ-UHFFFAOYSA-N 0.000 description 2
- LACNYRKVXDENHB-UHFFFAOYSA-N 3a,4,5,7a-tetrahydroisoindole-1,3-dione;potassium Chemical compound [K].C1=CCCC2C(=O)NC(=O)C21 LACNYRKVXDENHB-UHFFFAOYSA-N 0.000 description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 2
- 229910011458 Li4/3 Ti5/3O4 Inorganic materials 0.000 description 2
- 229910010199 LiAl Inorganic materials 0.000 description 2
- 229910012506 LiSi Inorganic materials 0.000 description 2
- 239000002033 PVDF binder Substances 0.000 description 2
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 2
- 239000004743 Polypropylene Substances 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 239000006258 conductive agent Substances 0.000 description 2
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 2
- 239000000428 dust Substances 0.000 description 2
- 239000003792 electrolyte Substances 0.000 description 2
- 230000005764 inhibitory process Effects 0.000 description 2
- 239000011229 interlayer Substances 0.000 description 2
- BYXYCUABYHCYLY-UHFFFAOYSA-N isoindole-1,3-dione;potassium Chemical compound [K].C1=CC=C2C(=O)NC(=O)C2=C1 BYXYCUABYHCYLY-UHFFFAOYSA-N 0.000 description 2
- FHRJYLDOUAFOQS-UHFFFAOYSA-N isoindole-1,3-dione;potassium;pyridine Chemical compound [K].C1=CC=NC=C1.C1=CC=C2C(=O)NC(=O)C2=C1 FHRJYLDOUAFOQS-UHFFFAOYSA-N 0.000 description 2
- 238000012423 maintenance Methods 0.000 description 2
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 150000002891 organic anions Chemical class 0.000 description 2
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 2
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- 239000004926 polymethyl methacrylate Substances 0.000 description 2
- 229920001155 polypropylene Polymers 0.000 description 2
- 229920001296 polysiloxane Polymers 0.000 description 2
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 2
- 239000007774 positive electrode material Substances 0.000 description 2
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 2
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 1
- GAKRZMKKOYEPMZ-UHFFFAOYSA-N 3a,4,5,7a-tetrahydroisoindole-1,3-dione;calcium Chemical compound [Ca].C1=CCCC2C(=O)NC(=O)C21 GAKRZMKKOYEPMZ-UHFFFAOYSA-N 0.000 description 1
- QZHIJPDVQJDLSO-UHFFFAOYSA-N 3a,4,5,7a-tetrahydroisoindole-1,3-dione;magnesium Chemical compound [Mg].C1=CCCC2C(=O)NC(=O)C21 QZHIJPDVQJDLSO-UHFFFAOYSA-N 0.000 description 1
- NOUSRZCHFPFLJH-UHFFFAOYSA-N 3a,4,5,7a-tetrahydroisoindole-1,3-dione;sodium Chemical compound [Na].C1=CCCC2C(=O)NC(=O)C21 NOUSRZCHFPFLJH-UHFFFAOYSA-N 0.000 description 1
- RYSJBINQYKBLGC-UHFFFAOYSA-N 3a,4,5,7a-tetrahydroisoindole-1,3-dione;strontium Chemical compound [Sr].C1=CCCC2C(=O)NC(=O)C21 RYSJBINQYKBLGC-UHFFFAOYSA-N 0.000 description 1
- GCVIFIMEYPSFBB-UHFFFAOYSA-N 7a-ethyl-3ah-isoindole-1,3-dione;potassium Chemical compound [K].C1=CC=CC2C(=O)NC(=O)C21CC GCVIFIMEYPSFBB-UHFFFAOYSA-N 0.000 description 1
- 229910012820 LiCoO Inorganic materials 0.000 description 1
- 229910012851 LiCoO 2 Inorganic materials 0.000 description 1
- 229910015645 LiMn Inorganic materials 0.000 description 1
- 229910014689 LiMnO Inorganic materials 0.000 description 1
- 229910013290 LiNiO 2 Inorganic materials 0.000 description 1
- 229910013872 LiPF Inorganic materials 0.000 description 1
- 229910001290 LiPF6 Inorganic materials 0.000 description 1
- 229910013856 LiPb Inorganic materials 0.000 description 1
- 229910012381 LiSn Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 0.000 description 1
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- QOSMNYMQXIVWKY-UHFFFAOYSA-N Propyl levulinate Chemical compound CCCOC(=O)CCC(C)=O QOSMNYMQXIVWKY-UHFFFAOYSA-N 0.000 description 1
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 1
- CAELVZHFEPZQFD-UHFFFAOYSA-N [K].N1=CC=CC=C1.C(C)C12C(C(=O)NC1=O)C=CC=C2 Chemical compound [K].N1=CC=CC=C1.C(C)C12C(C(=O)NC1=O)C=CC=C2 CAELVZHFEPZQFD-UHFFFAOYSA-N 0.000 description 1
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- 239000000470 constituent Substances 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 150000004862 dioxolanes Chemical class 0.000 description 1
- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 1
- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical class CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- 210000003168 insulating cell Anatomy 0.000 description 1
- 229910001416 lithium ion Inorganic materials 0.000 description 1
- ACFSQHQYDZIPRL-UHFFFAOYSA-N lithium;bis(1,1,2,2,2-pentafluoroethylsulfonyl)azanide Chemical compound [Li+].FC(F)(F)C(F)(F)S(=O)(=O)[N-]S(=O)(=O)C(F)(F)C(F)(F)F ACFSQHQYDZIPRL-UHFFFAOYSA-N 0.000 description 1
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- 239000010935 stainless steel Substances 0.000 description 1
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- 239000000126 substance Substances 0.000 description 1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- 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
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
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- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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Abstract
本发明的非水电解质电池由金属锂、锂合金或可吸藏释放锂的材料形成的负极,正极,溶剂及溶于前述溶剂的溶质组成的非水电解质构成。前述非水电解质中包含选自酞酰亚胺、酞酰亚胺衍生物、酞酰亚胺啶、酞酰亚胺啶衍生物、四氢酞酰亚胺及四氢酞酰亚胺衍生物的至少1种添加剂。由于前述添加剂的作用,本发明的非水电解质电池即使在高温下长期保存也很难引起内部电阻的上升,对于二次电池来讲,还能够提高充放电循环特性。
Description
技术领域
本发明涉及非水电解质电池。本发明更具体涉及含有抑制电池内部电阻上升的添加剂的非水电解质。
背景技术
近年,随着电器产品的小型化和轻量化,对产品所用的具有高能量密度的电池的要求更高。对具有金属锂构成的负极的锂一次电池、具有碳材构成的负极的锂离子二次电池的研究正倍受瞩目。
上述电池中构成非水电解质的溶剂可使用碳酸亚丙酯、碳酸亚乙酯、碳酸亚丁酯、环丁砜、γ-丁内酯、碳酸二甲酯、碳酸二乙酯、1,2-二甲氧基乙烷、四氢呋喃、二氧戊环等,它们可单独使用,也可混合使用。此外,溶于溶剂的溶质可使用LiClO4、LiPF6、LiCF3SO3、LiN(CF3SO2)2、LiN(C2F5SO2)2等,它们可单独使用,也可混合使用。
最近,关于对包含凝胶状非水电解质和固体聚合物电解质的锂聚合物电池进行研究。凝胶状电解质中包含为保持上述溶质及溶剂而添加的主体聚合物。固体聚合物电解质是聚合物本身作为溶质的溶剂的电解质。例如,采用和包含在凝胶状非水电解质中的主体聚合物同样的聚合物。
构成这些电解质的聚合物可采用以聚偏二氟乙烯、聚环氧乙烷、聚丙烯腈、聚甲基丙烯酸甲酯、聚硅氧烷等为主体的衍生物。
众所周知,上述非水电解质的构成要素会和电池内的水分及电极,甚至隔层的构成材料发生化学反应。特别是构成负极的金属锂、LiAl、LiSi等锂合金及能够吸藏释放锂的碳材和非水电解质构成要素的反应性较高,通过化学反应等会在负极表面生成有机物薄膜。这种现象在高温下,特别是80℃以上的温度下保存电池后,或反复对二次电池进行充放电循环时容易发生。非水电解质电池中作为正极活性物质所用的大多数金属氧化物都溶于非水电解质,溶解的物质析出在负极表面上,这种现象就可确认形成了薄膜。
由于这些薄膜的导电性较低,所以是导致电池内部电阻上升的原因之一。电池的保存时间如果过长,则电池内部电阻的上升会使放电时的电压下降增加,不能够获得充分的放电特性。即使反复对二次电池进行充放电循环,也同样存在电池内部电阻上升,循环特性受损的问题。
于是提出了通过在非水电解质中添加会在负极表面形成薄膜的添加剂以抑制电池内部电阻上升的方法。如日本专利公开公报平7-22069号所述,这类添加剂包括芳香族二羧酸酯等。但是,这些添加剂对室温保存时的电池虽然有效,对经过高温保存或反复进行过充放电循环的电池却无效。
本发明的目的是防止非水电解质电池在高温保存时因化学反应而在负极表面形成有机物薄膜,抑制一次电池及二次电池内部电阻的上升,并使二次电池的充放电循环特性有所提高。
发明的揭示
本发明的非水电解质电池具备金属锂、锂合金或可吸藏释放锂的材料形成的负极,正极,溶剂及溶于前述溶剂的溶质组成的非水电解质,前述非水电解质中包含选自通式(1):表示的化合物(X1~X4分别为独立的氢原子、F、Cl、Br、I或碳原子数1~3的烷基,Y1为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,i为1或2),通式(2):表示的化合物(X5~X8分别为独立的氢原子、F、Cl、Br、I或碳原子数1~3的烷基,Y2为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,j为1或2),通式(3):表示的化合物(Y3为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,k为1或2)的至少1种添加剂。
前述非水电解质中,对应于前述溶剂及前述溶质的合计量,前述添加剂的含量较好为0.001~10重量%。
前述溶质较好为选自LiPF6、LiBF4、LiCiO4、LiCF3SO3、LiAsF6、通式(4):LiN(CmX9 2m+1Z1)2表示的锂盐、通式(5):LiC(CnX10 2n+1Z2)3表示的锂盐及通式(6):LiCR(CpX11 2p+1Z3)2表示的锂盐(X9~X11分别为独立的F、Cl、Br或I,m、n和p分别为独立的1~4的整数,Z1~Z3分别为独立的CO或SO2)的至少1种。
前述溶剂包含选自碳酸亚乙酯、碳酸亚丙酯、碳酸亚丁酯及γ-丁内酯的至少1种。
对附图的简单说明
图1为表示本发明的非水电解质电池的结构纵截面图。
实施发明的最佳方式
本发明的非水电解质电池中的非水电解质包括液状非水电解质及凝胶状非水电解质。液状非水电解质中包含作为溶剂的有机溶剂。凝胶状非水电解质一般由前述液状非水电解质和保持该电解质的主体聚合物组成。本发明的特征就是在这些非水电解质中添加了添加剂。
即,本发明的非水电解质电池中的非水电解质包含选自通式(1):表示的化合物(X1~X4分别为独立的氢原子、F、Cl、Br、I或碳原子数1~3的烷基,Y1为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,i为1或2)(酞酰亚胺或其衍生物),通式(2):表示的化合物(X5~X8分别为独立的氢原子、F、Cl、Br、I或碳原子数1~3的烷基,Y2为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,j为1或2)(酞酰亚胺啶或其衍生物),通式(3):表示的化合物(Y3为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,k为1或2)(四氢酞酰亚胺或其衍生物)的至少1种添加剂。
选自X1~X8的至少1个为氢原子以外的基团,其余为氢原子时,氢原子以外的基团最好为烷基或氟原子。
X1~X4中的1个为烷基,其他为氢原子时,X2或X3最好为烷基。此外,X5~X8中的1个为烷基,其他为氢原子时,X6或X7最好为烷基,特别好的是X6为烷基。上述任何情况下,作为烷基最好为乙基。
此外,X1~X4中的2个为氟原子,其他为氢原子时,X2及X3最好为氟原子。X5~X8中的2个为氟原子,其他为氢原子时,X6及X7最好为氟原子。
通式(1)~(3)中,Y1~Y3为2价原子,例如,Mg、Ca、Sr或Ba时,前述添加剂具有2个有机阴离子,这2个有机阴离子可以相同也可以不同。
通式(1)~(3)表示的化合物比作为非水电解质构成要素的有机溶剂更优先与负极反应,在负极表面上形成具有和酞酰亚胺、酞酰亚胺啶等结构相近的稳定薄膜,抑制有机溶剂和负极的反应。而且,形成的薄膜具有良好的锂离子导电性,象传统添加剂那样基本不会使电池内部电阻上升。
通式(1)~(3)表示的化合物包括酞酰亚胺、2-乙基酞酰亚胺、2-氟酞酰亚胺、酞酰亚胺钾、2-乙基酞酰亚胺钾、2-氟酞酰亚胺钾、酞酰亚胺啶、2-乙基酞酰亚胺啶、2-氟酞酰亚胺啶、酞酰亚胺啶钾、2-乙基酞酰亚胺啶钾、2-氟酞酰亚胺啶钾、四氢酞酰亚胺、四氢酞酰亚胺钠、四氢酞酰亚胺钾、四氢酞酰亚胺镁、四氢酞酰亚胺钙、四氢酞酰亚胺锶等。
其中,酞酰亚胺、2-乙基酞酰亚胺、2-氟酞酰亚胺、酞酰亚胺啶、2-乙基酞酰亚胺啶、2-氟酞酰亚胺啶、四氢酞酰亚胺、四氢酞酰亚胺钾不仅在负极表面形成的薄膜稳定性增加,而且和正极、负极及非水电解质的溶剂和溶质的反应性较低,可以说这些化合物是最理想的。
非水电解质中,对应于前述溶剂和前述溶质的合计量,前述添加剂的量一般为0.001~10重量%,更好为0.001~1重量%。
前述溶质可采用LiClO4、LiPF6、LiBF4、LiCF3SO3、LiN(CF3SO2)2、LiN(C2F5SO2)2、LiN(CF3SO2)(C4F9SO2)等。它们可单独使用,也可2种以上混合使用。非水电解质中的溶质浓度较好是在0.2~2.0摩尔/升的范围内。
构成液状非水电解质的有机溶剂可采用碳酸亚乙酯、碳酸亚丙酯、碳酸亚丁酯、γ-丁内酯、环丁砜、碳酸亚乙烯酯等介电常数较高的有机溶剂和碳酸二甲酯、碳酸乙基甲酯、碳酸二乙酯、1,2-二甲氧基乙烷等低粘度有机溶剂的混合物。特别好的是包含选自碳酸亚乙酯、碳酸亚丙酯、碳酸亚丁酯及γ-丁内酯的至少1种有机溶剂。
凝胶状非水电解质的主体聚合物包括以聚偏二氟乙烯、聚环氧乙烷、聚丙烯腈、聚甲基丙烯酸甲酯、聚硅氧烷等为主体的衍生物。
通过将上述非水电解质和规定的正极、负极组合在一起,能够获得即使在高温条件下长期保存也难以使电池内部电阻上升的一次电池、在高温条件下也具备良好充放电循环特性的二次电池。
正极可采用以往用于非水电解质电池正极的材料制得。正极材料包括LiCoO2、LiNiO2、LiMn2O4、LiMnO2、V2O5、V6O13、MnO2、WO3、Nb2O5、Li4/3Ti5/3O4等金属氧化物,CFx(x≤1)表示的氟化碳,FeS2、TiS2等硫化物,以及聚吡咯和聚苯胺等导电性聚合物。
负极可采用以往用于非水电解质电池负极的材料制得。负极材料包括金属锂,LiAl、LiSi、LiSn、LiNiSi、LiPb等锂合金,可吸藏释放锂的石墨,焦炭等碳材,SiO、SnO、Fe2O3、WO2、Nb2O5、Li4/3Ti5/3O4等金属氧化物,Li0.4CoN等氮化物。
以下,以实施例为基础对本发明进行具体说明。
实施例1
图1为本实施例所用的硬币形电池的纵截面图。2和6分别表示不锈钢制正极外壳和负极外壳。5表示聚丙烯制绝缘衬垫。1为正极、4为负极。3为聚丙烯制非织造布组成的隔层。该电池的尺寸是外径20mm、高2.5mm。
按照80∶10∶10的重量比混合作为正极活性物质的LiCoO2粉末、作为导电剂的碳粉及作为粘合剂的含氟树脂后,干燥获得正极合剂。以2ton/cm2的压力对该正极合剂加压使其成形为直径16mm、厚度0.9mm的颗粒,然后在水分1%以下的干燥氛围气中于250℃干燥,获得正极。
另一方面,按照85∶15的重量比混合作为负极活性物质的天然石墨粉末和作为粘合剂的含氟树脂,获得负极合剂。以2ton/cm2的压力对该负极合剂加压使其成形为直径16mm、厚度0.9mm的颗粒,然后在水分1%以下的干燥氛围气中于110℃干燥,获得负极。
按照5∶5的体积比混合碳酸亚乙酯和碳酸二乙酯,获得非水电解质的溶剂,然后以1.0摩尔/升的比例在其中溶解作为溶质的LiPF6。对应于前述溶剂和LiPF6的合计重量,以0.1重量%的比例在所得非水电解质中添加表1所示的添加剂A1、B1、C1或D1,表2所示的添加剂A2、B2、C2或D2,或表3所示的A3或B3。
表2
表3
采用所得包含添加剂的非水电解质、正极及负极,制得前述硬币形电池A1、B1、C1、D1、A2、B2、C2、D2、A3及B3。在电池内注入非水电解质100mg。
作为比较例,采用不含添加剂的非水电解质,制得同样的电池1。
以下,对各电池进行评估。
在1mA/cm2的额定电流下对电池进行充电使电压达到4.2V,测定电池的内部电阻。然后,将处于充电状态的电池A1~D1、A2~D2及电池1放置在60℃的恒温槽内,历时2个月,将电池A3及B3放置在85℃的恒温槽内,历时20天,测定保存后的电池内部电阻。以1kHz的交流电测定内部电阻,其结果如表4所示。
表4
电池 | 添加剂 | 电池内部电阻(Ω) | ||
保存前 | 保存后 | 充放电循环后 | ||
电池A1 | A1 | 12.3 | 14.1 | 14.4 |
电池B1 | B1 | 13.0 | 14.4 | 14.6 |
电池C1 | C1 | 12.2 | 12.5 | 12.7 |
电池D1 | D1 | 12.1 | 12.3 | 12.4 |
电池A2 | A2 | 12.8 | 14.2 | 14.5 |
电池B2 | B2 | 13.5 | 14.5 | 14.7 |
电池C2 | C2 | 12.7 | 12.9 | 13.3 |
电池D2 | D2 | 12.6 | 12.7 | 13.1 |
电池A3 | A3 | 12.5 | 14.2 | 14.8 |
电池B3 | B3 | 13.3 | 14.6 | 15.0 |
电池1 | 无 | 11.3 | 20.4 | 21.2 |
另一方面,以1mA/cm2的额定电流,在3.0~4.2V的电压范围内,对电池反复进行100次充放电循环后,测定电池的内部电阻,其结果如表4所示。
表4中,任何加入了添加剂的电池的内部电阻都比未加入添加剂的电池1稳定,经高温下保存及充放电循环后的内部电阻上升也较少。
此外,上述添加剂中,添加了添加剂D1、D2的电池显现出最好的结果。
实施例2
本实施例中图1所示结构的钮扣形电池的制作方法如下所述。
以80∶10∶10的重量比混合经过400℃的加热处理的电解二氧化锰、作为导电剂的碳粉和作为粘合剂的含氟树脂,获得正极合剂。以2ton/cm2的压力对该正极合剂加压使其成形为直径16mm的颗粒,然后在水分1%以下的干燥氛围气中于250℃干燥,获得正极。
负极由金属锂构成。即,按照规定尺寸对锂压延板进行冲孔落料,然后将其固定在负极外壳6的内面。
按照5∶5的体积比混合碳酸亚丙酯和1,2-二甲氧基乙烷,获得非水电解质的溶剂,然后以1.0摩尔/升的比例在其中溶解作为溶质的LiCF3SO3。对应于前述溶剂和LiCF3SO3的合计重量,以0.1重量%的比例在所得非水电解质中添加表1所示的添加剂A1、B1、C1或D1,表2所示的添加剂A2、B2、C2或D2,或表3所示的A3或B3。
采用所得非水电解质、正极及负极,制得前述硬币形电池A1’、B1’、C1’、D1’、A2’、B2’、C2’、D2’、A3’及B3’。在电池内注入非水电解质160mg。
作为比较例,采用不含添加剂的非水电解质,制得同样的电池2。
以下,对各电池进行评估。
测定电池的内部电阻后,将电池A1’~D1’、A2’~D2’及电池2放置在60℃的恒温槽内,历时2个月,将电池A3’及B3’放置在85℃的恒温槽内,历时20天,测定保存后的电池内部电阻。以1kHz的交流电测定内部电阻,其结果如表5所示。
表5
电池 | 添加剂 | 电池内部电阻(Ω) | |
保存前 | 保存后 | ||
电池A1’ | A1 | 10.1 | 11.4 |
电池B1’ | B1 | 9.1 | 10.1 |
电池C1’ | C1 | 8.6 | 9.2 |
电池D1’ | D1 | 8.4 | 8.9 |
电池A2’ | A2 | 10.6 | 11.3 |
电池B2’ | B2 | 9.8 | 10.1 |
电池C2’ | C2 | 9.2 | 9.5 |
电池D2’ | D2 | 8.9 | 9.1 |
电池A3’ | A3 | 10.5 | 13.3 |
电池B3’ | B3 | 9.8 | 12.8 |
电池2 | 无 | 8.2 | 15.3 |
表5中,任何加入了添加剂的电池的内部电阻都比未加入添加剂的电池2稳定,经高温下保存后的内部电阻上升也较少。
实施例3
除了对应于前述溶剂和LiCF3SO3的合计重量,添加剂D1的添加比例为0.0005~15重量%之外,其他都和实施例2中的电池D1’相同,制得同样的电池。然后,和实施例2的电池D1’进行同样的评估,其结果如表6所示。
表6
D1的添加量(重量%) | 电池内部电阻(Ω) | |
保存前 | 保存后 | |
0 | 8.2 | 15.3 |
0.0005 | 8.2 | 13.9 |
0.001 | 8.3 | 9.2 |
0.01 | 8.3 | 9.0 |
0.1 | 8.4 | 8.9 |
1.0 | 8.6 | 9.3 |
10 | 8.8 | 9.7 |
15 | 13.1 | 14.6 |
除了对应于前述溶剂和LiCF3SO3的合计重量,添加剂D2的添加比例为0.0005~15重量%之外,其他都和实施例2中的电池D2’相同,制得同样的电池。然后,和实施例2的电池D2’进行同样的评估,其结果如表7所示。
表7
D2的添加量(重量%) | 电池内部电阻(Ω) | |
保存前 | 保存后 | |
0 | 8.2 | 15.3 |
0.0005 | 8.3 | 13.2 |
0.001 | 8.5 | 9.3 |
0.01 | 8.6 | 8.9 |
0.1 | 8.9 | 9.1 |
1.0 | 9.1 | 9.3 |
10 | 9.5 | 9.9 |
15 | 13.6 | 14.9 |
除了对应于前述溶剂和LiCF3SO3的合计重量,添加剂A3的添加比例为0.0005~15重量%之外,其他都和实施例2中的电池A3’相同,制得同样的电池。然后,和实施例2的电池A3’进行同样的评估,其结果如表8所示。
表8
A3的添加量(重量%) | 电池内部电阻(Ω) | |
保存前 | 保存后 | |
0 | 8.2 | 21.5 |
0.0005 | 8.5 | 19.8 |
0.001 | 8.9 | 15.2 |
0.01 | 9.6 | 13.8 |
0.1 | 10.5 | 13.3 |
1.0 | 10.8 | 13.3 |
10 | 12.5 | 14.5 |
15 | 13.8 | 17.2 |
表6~表8中,对应于溶剂和LiCF3SO3的合计量,添加剂的添加比例在0.001~10.0重量%的范围内,尤其抑制了内部电阻的上升。
对应于溶剂和LiCF3SO3的合计量,添加剂的添加比例如果不足0.001重量%,则抑制内部电阻上升的效果发挥就不充分。另一方面,如果添加比例超过10.0重量%,则添加剂本身会导致内部电阻的上升。此外,当添加比例在0.01~1.0重量%的范围内时,能够显现出最好的结果。另外,使用除D1、D2及A3以外的添加剂,并进行同样的评估时也有同样的倾向。
实施例3中,对一次电池的本发明效果进行了说明,但为二次电池时,不仅能够抑制高温保存时内部电阻的上升,还能够使充放电循环特性有所提高。
上述各实施例中,虽然仅制作了硬币形电池。但本发明也同样适用于圆筒形电池、方形电池及其他形状的电池。
以上实施例中,虽然仅对液状非水电解质进行了说明,但本发明也同样适用于使用了凝胶状非水电解质和固体聚合物电解质的电池。
产业上利用的可能性
利用本发明能够获得即使在高温条件下长期保存也很难使内部电阻上升的非水电解质电池。对于二次电池,还能够提高其充放电循环特性。
Claims (4)
1.非水电解质电池,所述电池由金属锂、锂合金或可吸藏释放锂的材料形成的负极,正极,溶剂及溶于前述溶剂的溶质组成的非水电解质构成,前述非水电解质中包含选自通式(1):表示的化合物(X1~X4分别为独立的氢原子、F、Cl、Br、I或碳原子数1~3的烷基,Y1为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,i为1或2),通式(2):表示的化合物(X5~X8分别为独立的氢原子、F、Cl、Br、I或碳原子数1~3的烷基,Y2为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,j为1或2),通式(3):表示的化合物(Y3为氢原子、Na、K、Rb、Cs、Mg、Ca、Sr或Ba,k为1或2)的至少1种添加剂。
2.如权利要求1所述的非水电解质电池,其中,对应于前述溶剂及前述溶质的合计量,前述非水电解质中的前述添加剂的含量为0.001~10重量%。
3.如权利要求1所述的非水电解质电池,其中,前述溶质为选自LiPF6、LiBF4、LiClO4、LiCF3SO3、LiAsF6、通式(4):LiN(CmX9 2m+1Z1)2表示的锂盐、通式(5):LiC(CnX10 2n+1Z2)3表示的锂盐及通式(6):LiCR(CpX11 2p+1Z3)2表示的锂盐(X9~X11分别为独立的F、Cl、Br或I,m、n和p分别为独立的1~4的整数,Z1~Z3分别为独立的CO或SO2)的至少1种。
4.如权利要求1所述的非水电解质电池,其中,前述溶剂包含选自碳酸亚乙酯、碳酸亚丙酯、碳酸亚丁酯及γ-丁内酯的至少1种。
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JP337131/1999 | 1999-11-29 | ||
JP33713099 | 1999-11-29 | ||
JP33713199 | 1999-11-29 | ||
JP337130/1999 | 1999-11-29 | ||
JP2000325310 | 2000-10-25 | ||
JP325310/2000 | 2000-10-25 |
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CN1338129A true CN1338129A (zh) | 2002-02-27 |
CN1174515C CN1174515C (zh) | 2004-11-03 |
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US (1) | US6641957B1 (zh) |
EP (1) | EP1209754B1 (zh) |
JP (1) | JP3720300B2 (zh) |
KR (1) | KR100414718B1 (zh) |
CN (1) | CN1174515C (zh) |
TW (1) | TW475295B (zh) |
WO (1) | WO2001041247A1 (zh) |
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CN1321994C (zh) * | 2005-09-23 | 2007-06-20 | 南开大学 | 1,2,3,6-四氢酞酰亚胺类化合物及其制备和用途 |
CN100376057C (zh) * | 2004-07-07 | 2008-03-19 | 比亚迪股份有限公司 | 一种非水电解液锂离子二次电池 |
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JP4590685B2 (ja) * | 2000-05-10 | 2010-12-01 | 三菱化学株式会社 | リチウム二次電池用正極材料、リチウム二次電池用正極及びリチウム二次電池 |
JP4288400B2 (ja) * | 2001-11-15 | 2009-07-01 | 日本電気株式会社 | 二次電池用電解液の製造方法および二次電池用電解液、二次電池の製造方法および二次電池 |
US20040229127A1 (en) | 2003-05-13 | 2004-11-18 | Wensley C. Glen | Polyimide matrix electrolyte |
US20040253520A1 (en) * | 2003-05-13 | 2004-12-16 | Wensley C. Glen | Polyimide matrix electrolyte and improved batteries therefrom |
US6936377B2 (en) * | 2003-05-13 | 2005-08-30 | C. Glen Wensley | Card with embedded IC and electrochemical cell |
US7390336B2 (en) * | 2003-07-29 | 2008-06-24 | Solicore, Inc. | Polyimide-based lithium metal battery |
US20050048369A1 (en) * | 2003-08-28 | 2005-03-03 | Matsushita Electric Industrial Co., Ltd. | Negative electrode for non-aqueous electrolyte secondary battery, production method thereof and non-aqueous electrolyte secondary battery |
JP4404594B2 (ja) * | 2003-09-29 | 2010-01-27 | 三洋電機株式会社 | 非水電解質二次電池 |
EP3176857A1 (en) | 2004-07-22 | 2017-06-07 | BrightVolt, Inc. | Improved battery tab and packaging design |
JP4753690B2 (ja) * | 2004-11-18 | 2011-08-24 | パナソニック株式会社 | 有機電解質電池 |
JP2006236889A (ja) * | 2005-02-28 | 2006-09-07 | Matsushita Electric Ind Co Ltd | 非水電解液一次電池 |
JP4396675B2 (ja) * | 2006-06-16 | 2010-01-13 | ソニー株式会社 | 非水電解質二次電池 |
US9123971B2 (en) | 2010-09-02 | 2015-09-01 | Nec Corporation | Secondary battery |
JP5830689B2 (ja) * | 2010-11-12 | 2015-12-09 | パナソニックIpマネジメント株式会社 | リチウム一次電池 |
JP6271275B2 (ja) * | 2014-02-05 | 2018-01-31 | Fdk株式会社 | リチウム一次電池用非水系有機電解液、およびリチウム一次電池 |
JP2021180064A (ja) * | 2018-08-02 | 2021-11-18 | パナソニックIpマネジメント株式会社 | リチウム一次電池 |
CN110707310B (zh) * | 2019-10-29 | 2021-01-12 | 昆山宝创新能源科技有限公司 | 负极材料及其制备方法和应用 |
JP7313021B2 (ja) * | 2020-01-20 | 2023-07-24 | パナソニックIpマネジメント株式会社 | リチウム一次電池およびリチウム一次電池用非水電解液 |
JP7530015B2 (ja) | 2021-01-12 | 2024-08-07 | 日本電信電話株式会社 | リチウム二次電池の製造方法 |
WO2023162917A1 (ja) * | 2022-02-22 | 2023-08-31 | パナソニックIpマネジメント株式会社 | リチウム一次電池 |
WO2024043273A1 (ja) * | 2022-08-24 | 2024-02-29 | パナソニックIpマネジメント株式会社 | リチウム一次電池 |
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- 2000-11-28 KR KR10-2001-7009330A patent/KR100414718B1/ko active IP Right Grant
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Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
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CN100376057C (zh) * | 2004-07-07 | 2008-03-19 | 比亚迪股份有限公司 | 一种非水电解液锂离子二次电池 |
CN1321994C (zh) * | 2005-09-23 | 2007-06-20 | 南开大学 | 1,2,3,6-四氢酞酰亚胺类化合物及其制备和用途 |
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EP1209754A4 (en) | 2005-10-05 |
TW475295B (en) | 2002-02-01 |
KR20020018646A (ko) | 2002-03-08 |
KR100414718B1 (ko) | 2004-01-13 |
CN1174515C (zh) | 2004-11-03 |
JP3720300B2 (ja) | 2005-11-24 |
EP1209754A1 (en) | 2002-05-29 |
US6641957B1 (en) | 2003-11-04 |
EP1209754B1 (en) | 2011-10-05 |
WO2001041247A1 (fr) | 2001-06-07 |
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