WO2005071703A1 - キャパシタ用セパレーターおよびキャパシタ - Google Patents
キャパシタ用セパレーターおよびキャパシタ Download PDFInfo
- Publication number
- WO2005071703A1 WO2005071703A1 PCT/JP2005/001292 JP2005001292W WO2005071703A1 WO 2005071703 A1 WO2005071703 A1 WO 2005071703A1 JP 2005001292 W JP2005001292 W JP 2005001292W WO 2005071703 A1 WO2005071703 A1 WO 2005071703A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- electric double
- double layer
- layer capacitor
- separator
- electrolyte
- Prior art date
Links
- 239000003990 capacitor Substances 0.000 title claims abstract description 59
- 239000004760 aramid Substances 0.000 claims abstract description 31
- 229920003235 aromatic polyamide Polymers 0.000 claims abstract description 31
- 230000035699 permeability Effects 0.000 claims abstract description 10
- 239000012528 membrane Substances 0.000 claims description 42
- 239000003792 electrolyte Substances 0.000 claims description 24
- 229920000642 polymer Polymers 0.000 claims description 19
- 239000002904 solvent Substances 0.000 claims description 17
- 239000011255 nonaqueous electrolyte Substances 0.000 claims description 16
- 150000001408 amides Chemical class 0.000 claims description 13
- 239000011148 porous material Substances 0.000 claims description 10
- 150000003863 ammonium salts Chemical class 0.000 claims description 7
- 238000010438 heat treatment Methods 0.000 claims description 7
- 239000002608 ionic liquid Substances 0.000 claims description 7
- 239000003125 aqueous solvent Substances 0.000 claims description 6
- 238000005345 coagulation Methods 0.000 claims description 6
- 230000015271 coagulation Effects 0.000 claims description 6
- QZUPTXGVPYNUIT-UHFFFAOYSA-N isophthalamide Chemical compound NC(=O)C1=CC=CC(C(N)=O)=C1 QZUPTXGVPYNUIT-UHFFFAOYSA-N 0.000 claims description 4
- 239000007788 liquid Substances 0.000 claims description 4
- 238000000926 separation method Methods 0.000 claims description 4
- 239000000126 substance Substances 0.000 claims description 4
- 238000005406 washing Methods 0.000 claims description 4
- 239000004952 Polyamide Substances 0.000 claims description 3
- 229920002647 polyamide Polymers 0.000 claims description 3
- 239000003660 carbonate based solvent Substances 0.000 claims 1
- 239000012046 mixed solvent Substances 0.000 claims 1
- 230000010220 ion permeability Effects 0.000 abstract description 2
- -1 aromatic dicarboxylic acid halide Chemical class 0.000 description 24
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 11
- SECXISVLQFMRJM-UHFFFAOYSA-N N-Methylpyrrolidone Chemical compound CN1CCCC1=O SECXISVLQFMRJM-UHFFFAOYSA-N 0.000 description 10
- 239000000243 solution Substances 0.000 description 9
- 150000002500 ions Chemical class 0.000 description 8
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 6
- 230000014759 maintenance of location Effects 0.000 description 6
- 238000000034 method Methods 0.000 description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 4
- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 4
- 150000001450 anions Chemical class 0.000 description 4
- 150000004984 aromatic diamines Chemical class 0.000 description 4
- 150000001768 cations Chemical class 0.000 description 4
- 239000008151 electrolyte solution Substances 0.000 description 4
- QQVIHTHCMHWDBS-UHFFFAOYSA-N isophthalic acid Chemical compound OC(=O)C1=CC=CC(C(O)=O)=C1 QQVIHTHCMHWDBS-UHFFFAOYSA-N 0.000 description 4
- 230000000704 physical effect Effects 0.000 description 4
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 4
- 239000004810 polytetrafluoroethylene Substances 0.000 description 4
- WZCQRUWWHSTZEM-UHFFFAOYSA-N 1,3-phenylenediamine Chemical compound NC1=CC=CC(N)=C1 WZCQRUWWHSTZEM-UHFFFAOYSA-N 0.000 description 3
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- 239000004743 Polypropylene Substances 0.000 description 3
- 229920002678 cellulose Polymers 0.000 description 3
- 239000001913 cellulose Substances 0.000 description 3
- 229920006254 polymer film Polymers 0.000 description 3
- 229920001155 polypropylene Polymers 0.000 description 3
- 239000000047 product Substances 0.000 description 3
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
- CBCKQZAAMUWICA-UHFFFAOYSA-N 1,4-phenylenediamine Chemical compound NC1=CC=C(N)C=C1 CBCKQZAAMUWICA-UHFFFAOYSA-N 0.000 description 2
- HLBLWEWZXPIGSM-UHFFFAOYSA-N 4-Aminophenyl ether Chemical compound C1=CC(N)=CC=C1OC1=CC=C(N)C=C1 HLBLWEWZXPIGSM-UHFFFAOYSA-N 0.000 description 2
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 2
- OFOBLEOULBTSOW-UHFFFAOYSA-N Malonic acid Chemical compound OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 2
- 125000003118 aryl group Chemical group 0.000 description 2
- 238000005266 casting Methods 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
- NAQMVNRVTILPCV-UHFFFAOYSA-N hexane-1,6-diamine Chemical compound NCCCCCCN NAQMVNRVTILPCV-UHFFFAOYSA-N 0.000 description 2
- 238000004519 manufacturing process Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 239000004745 nonwoven fabric Substances 0.000 description 2
- XNGIFLGASWRNHJ-UHFFFAOYSA-N phthalic acid Chemical compound OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 description 2
- 238000006068 polycondensation reaction Methods 0.000 description 2
- 230000002265 prevention Effects 0.000 description 2
- ZXMGHDIOOHOAAE-UHFFFAOYSA-N 1,1,1-trifluoro-n-(trifluoromethylsulfonyl)methanesulfonamide Chemical compound FC(F)(F)S(=O)(=O)NS(=O)(=O)C(F)(F)F ZXMGHDIOOHOAAE-UHFFFAOYSA-N 0.000 description 1
- VAYTZRYEBVHVLE-UHFFFAOYSA-N 1,3-dioxol-2-one Chemical compound O=C1OC=CO1 VAYTZRYEBVHVLE-UHFFFAOYSA-N 0.000 description 1
- YFOOEYJGMMJJLS-UHFFFAOYSA-N 1,8-diaminonaphthalene Chemical compound C1=CC(N)=C2C(N)=CC=CC2=C1 YFOOEYJGMMJJLS-UHFFFAOYSA-N 0.000 description 1
- LXJLFVRAWOOQDR-UHFFFAOYSA-N 3-(3-aminophenoxy)aniline Chemical compound NC1=CC=CC(OC=2C=C(N)C=CC=2)=C1 LXJLFVRAWOOQDR-UHFFFAOYSA-N 0.000 description 1
- NDXGRHCEHPFUSU-UHFFFAOYSA-N 3-(3-aminophenyl)aniline Chemical group NC1=CC=CC(C=2C=C(N)C=CC=2)=C1 NDXGRHCEHPFUSU-UHFFFAOYSA-N 0.000 description 1
- LJGHYPLBDBRCRZ-UHFFFAOYSA-N 3-(3-aminophenyl)sulfonylaniline Chemical compound NC1=CC=CC(S(=O)(=O)C=2C=C(N)C=CC=2)=C1 LJGHYPLBDBRCRZ-UHFFFAOYSA-N 0.000 description 1
- ZBMISJGHVWNWTE-UHFFFAOYSA-N 3-(4-aminophenoxy)aniline Chemical compound C1=CC(N)=CC=C1OC1=CC=CC(N)=C1 ZBMISJGHVWNWTE-UHFFFAOYSA-N 0.000 description 1
- GSYIVQLTSZFJRV-UHFFFAOYSA-N 3-(4-carboxyphenyl)benzoic acid Chemical compound C1=CC(C(=O)O)=CC=C1C1=CC=CC(C(O)=O)=C1 GSYIVQLTSZFJRV-UHFFFAOYSA-N 0.000 description 1
- CKOFBUUFHALZGK-UHFFFAOYSA-N 3-[(3-aminophenyl)methyl]aniline Chemical compound NC1=CC=CC(CC=2C=C(N)C=CC=2)=C1 CKOFBUUFHALZGK-UHFFFAOYSA-N 0.000 description 1
- LBPVOEHZEWAJKQ-UHFFFAOYSA-N 3-[4-(3-aminophenoxy)phenoxy]aniline Chemical compound NC1=CC=CC(OC=2C=CC(OC=3C=C(N)C=CC=3)=CC=2)=C1 LBPVOEHZEWAJKQ-UHFFFAOYSA-N 0.000 description 1
- ICNFHJVPAJKPHW-UHFFFAOYSA-N 4,4'-Thiodianiline Chemical compound C1=CC(N)=CC=C1SC1=CC=C(N)C=C1 ICNFHJVPAJKPHW-UHFFFAOYSA-N 0.000 description 1
- YBRVSVVVWCFQMG-UHFFFAOYSA-N 4,4'-diaminodiphenylmethane Chemical compound C1=CC(N)=CC=C1CC1=CC=C(N)C=C1 YBRVSVVVWCFQMG-UHFFFAOYSA-N 0.000 description 1
- NEQFBGHQPUXOFH-UHFFFAOYSA-N 4-(4-carboxyphenyl)benzoic acid Chemical compound C1=CC(C(=O)O)=CC=C1C1=CC=C(C(O)=O)C=C1 NEQFBGHQPUXOFH-UHFFFAOYSA-N 0.000 description 1
- ZYEDGEXYGKWJPB-UHFFFAOYSA-N 4-[2-(4-aminophenyl)propan-2-yl]aniline Chemical compound C=1C=C(N)C=CC=1C(C)(C)C1=CC=C(N)C=C1 ZYEDGEXYGKWJPB-UHFFFAOYSA-N 0.000 description 1
- WUPRYUDHUFLKFL-UHFFFAOYSA-N 4-[3-(4-aminophenoxy)phenoxy]aniline Chemical compound C1=CC(N)=CC=C1OC1=CC=CC(OC=2C=CC(N)=CC=2)=C1 WUPRYUDHUFLKFL-UHFFFAOYSA-N 0.000 description 1
- JCRRFJIVUPSNTA-UHFFFAOYSA-N 4-[4-(4-aminophenoxy)phenoxy]aniline Chemical compound C1=CC(N)=CC=C1OC(C=C1)=CC=C1OC1=CC=C(N)C=C1 JCRRFJIVUPSNTA-UHFFFAOYSA-N 0.000 description 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 description 1
- MQJKPEGWNLWLTK-UHFFFAOYSA-N Dapsone Chemical compound C1=CC(N)=CC=C1S(=O)(=O)C1=CC=C(N)C=C1 MQJKPEGWNLWLTK-UHFFFAOYSA-N 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 1
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical compound NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 description 1
- VZCYOOQTPOCHFL-OWOJBTEDSA-N Fumaric acid Chemical compound OC(=O)\C=C\C(O)=O VZCYOOQTPOCHFL-OWOJBTEDSA-N 0.000 description 1
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- UCKMPCXJQFINFW-UHFFFAOYSA-N Sulphide Chemical compound [S-2] UCKMPCXJQFINFW-UHFFFAOYSA-N 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- 125000003368 amide group Chemical group 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- HFACYLZERDEVSX-UHFFFAOYSA-N benzidine Chemical group C1=CC(N)=CC=C1C1=CC=C(N)C=C1 HFACYLZERDEVSX-UHFFFAOYSA-N 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- ZLSMCQSGRWNEGX-UHFFFAOYSA-N bis(4-aminophenyl)methanone Chemical compound C1=CC(N)=CC=C1C(=O)C1=CC=C(N)C=C1 ZLSMCQSGRWNEGX-UHFFFAOYSA-N 0.000 description 1
- DFFDSQBEGQFJJU-UHFFFAOYSA-M butyl carbonate Chemical compound CCCCOC([O-])=O DFFDSQBEGQFJJU-UHFFFAOYSA-M 0.000 description 1
- 238000003763 carbonization Methods 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 239000006258 conductive agent Substances 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000003851 corona treatment Methods 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 150000004985 diamines Chemical class 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- 208000028659 discharge Diseases 0.000 description 1
- JMLPVHXESHXUSV-UHFFFAOYSA-N dodecane-1,1-diamine Chemical compound CCCCCCCCCCCC(N)N JMLPVHXESHXUSV-UHFFFAOYSA-N 0.000 description 1
- 150000002170 ethers Chemical class 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 239000011888 foil Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 150000004676 glycans Chemical class 0.000 description 1
- 150000004820 halides Chemical class 0.000 description 1
- SYECJBOWSGTPLU-UHFFFAOYSA-N hexane-1,1-diamine Chemical compound CCCCCC(N)N SYECJBOWSGTPLU-UHFFFAOYSA-N 0.000 description 1
- 229910001416 lithium ion Inorganic materials 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 229940018564 m-phenylenediamine Drugs 0.000 description 1
- OKBVMLGZPNDWJK-UHFFFAOYSA-N naphthalene-1,4-diamine Chemical compound C1=CC=C2C(N)=CC=C(N)C2=C1 OKBVMLGZPNDWJK-UHFFFAOYSA-N 0.000 description 1
- KQSABULTKYLFEV-UHFFFAOYSA-N naphthalene-1,5-diamine Chemical compound C1=CC=C2C(N)=CC=CC2=C1N KQSABULTKYLFEV-UHFFFAOYSA-N 0.000 description 1
- VAWFFNJAPKXVPH-UHFFFAOYSA-N naphthalene-1,6-dicarboxylic acid Chemical compound OC(=O)C1=CC=CC2=CC(C(=O)O)=CC=C21 VAWFFNJAPKXVPH-UHFFFAOYSA-N 0.000 description 1
- JSKSILUXAHIKNP-UHFFFAOYSA-N naphthalene-1,7-dicarboxylic acid Chemical compound C1=CC=C(C(O)=O)C2=CC(C(=O)O)=CC=C21 JSKSILUXAHIKNP-UHFFFAOYSA-N 0.000 description 1
- RXOHFPCZGPKIRD-UHFFFAOYSA-N naphthalene-2,6-dicarboxylic acid Chemical compound C1=C(C(O)=O)C=CC2=CC(C(=O)O)=CC=C21 RXOHFPCZGPKIRD-UHFFFAOYSA-N 0.000 description 1
- HBJPJUGOYJOSLR-UHFFFAOYSA-N naphthalene-2,7-diamine Chemical compound C1=CC(N)=CC2=CC(N)=CC=C21 HBJPJUGOYJOSLR-UHFFFAOYSA-N 0.000 description 1
- WPUMVKJOWWJPRK-UHFFFAOYSA-N naphthalene-2,7-dicarboxylic acid Chemical compound C1=CC(C(O)=O)=CC2=CC(C(=O)O)=CC=C21 WPUMVKJOWWJPRK-UHFFFAOYSA-N 0.000 description 1
- 239000012466 permeate Substances 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 229920000139 polyethylene terephthalate Polymers 0.000 description 1
- 239000005020 polyethylene terephthalate Substances 0.000 description 1
- 229920005594 polymer fiber Polymers 0.000 description 1
- 229920001282 polysaccharide Polymers 0.000 description 1
- 239000005017 polysaccharide Substances 0.000 description 1
- 125000001453 quaternary ammonium group Chemical group 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- TYFQFVWCELRYAO-UHFFFAOYSA-N suberic acid Chemical compound OC(=O)CCCCCCC(O)=O TYFQFVWCELRYAO-UHFFFAOYSA-N 0.000 description 1
- 239000000758 substrate Substances 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- DZLFLBLQUQXARW-UHFFFAOYSA-N tetrabutylammonium Chemical compound CCCC[N+](CCCC)(CCCC)CCCC DZLFLBLQUQXARW-UHFFFAOYSA-N 0.000 description 1
- BJQWBACJIAKDTJ-UHFFFAOYSA-N tetrabutylphosphanium Chemical compound CCCC[P+](CCCC)(CCCC)CCCC BJQWBACJIAKDTJ-UHFFFAOYSA-N 0.000 description 1
- CBXCPBUEXACCNR-UHFFFAOYSA-N tetraethylammonium Chemical compound CC[N+](CC)(CC)CC CBXCPBUEXACCNR-UHFFFAOYSA-N 0.000 description 1
- SZWHXXNVLACKBV-UHFFFAOYSA-N tetraethylphosphanium Chemical compound CC[P+](CC)(CC)CC SZWHXXNVLACKBV-UHFFFAOYSA-N 0.000 description 1
- QEMXHQIAXOOASZ-UHFFFAOYSA-N tetramethylammonium Chemical compound C[N+](C)(C)C QEMXHQIAXOOASZ-UHFFFAOYSA-N 0.000 description 1
- BXYHVFRRNNWPMB-UHFFFAOYSA-N tetramethylphosphanium Chemical compound C[P+](C)(C)C BXYHVFRRNNWPMB-UHFFFAOYSA-N 0.000 description 1
- XOGCTUKDUDAZKA-UHFFFAOYSA-N tetrapropylphosphanium Chemical compound CCC[P+](CCC)(CCC)CCC XOGCTUKDUDAZKA-UHFFFAOYSA-N 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/52—Separators
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
- H01G11/58—Liquid electrolytes
- H01G11/60—Liquid electrolytes characterised by the solvent
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/54—Electrolytes
- H01G11/58—Liquid electrolytes
- H01G11/62—Liquid electrolytes characterised by the solute, e.g. salts, anions or cations therein
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/02—Diaphragms; Separators
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/13—Energy storage using capacitors
Definitions
- the present invention relates to a separator for an electric double layer capacitor which is excellent in high strength, high heat resistance, ion conductivity and electrolyte retention, and an electric double layer capacitor using the separator.
- the electrolyte When the electric double layer capacitor (hereinafter referred to as “capacitor”) is broadly classified, the electrolyte can be classified into aqueous electrolyte and non-aqueous electrolyte. Capacitors using non-aqueous electrolytes have approximately three times the energy density of capacitors using aqueous electrolytes, and are currently the mainstream electric double layer capacitors on the market.
- separators for capacitors paper separators made of cellulose and resin separators made of PTFE have been used.
- the separator In the case of a capacitor using a non-aqueous electrolyte, if the separator contains moisture, the electrical characteristics will be degraded. Therefore, the separator must be strictly dehydrated and dried.
- cellulose separators it is known that long-term heat treatment at a high temperature of 150 ° C or more causes carbonization of the cellulose, and drying at a temperature lower than 150 ° C is necessary. There is a problem that the drying time becomes longer.
- separator made of PTFE there is no problem from the viewpoint of removing moisture, but there is a problem in large-sized applications that handling is difficult due to low mechanical strength. Furthermore, separators made of PTFE are expensive and have not been developed for use in large quantities.
- JP-A-2003-272952 discloses that It has been proposed to use a nonwoven fabric made of a heat-resistant polymer fiber as a separator for a capacitor.
- nonwoven fabrics generally have defects called pinholes and have low electrolyte retention properties immediately.Thus, it is necessary to increase the film thickness or double the separator, which increases the internal resistance of the capacitor. Is not preferred. Disclosure of the invention
- the object of the present invention is to provide heat resistance and mechanical strength.
- DISCLOSURE OF THE INVENTION The present inventors have conducted intensive studies on the above-described problems, and have found that aromatic separators have been proposed to provide a separator for an electric double layer capacitor satisfying all ion permeability and an electric double layer capacitor using the separator.
- the present inventors have found that a porous membrane made of polyamide and controlled to a specific structure can realize a separator for electric double layer capacitors with excellent heat resistance, mechanical strength, ionic conductivity, and electrolyte solution retention. Arrives.
- the present invention is a porous film made of an aromatic polyamide and having a film thickness of 5 to 50 m, the porosity of the film is 30 to 80%, the air permeability is 5 to 300 seconds 1 OOmL-in 2 , and the unit is A separator for an electric double layer capacitor, wherein the piercing strength per film thickness is 50 mN / ⁇ m or more.
- the average pore size inside the porous membrane is preferably 0.01 to 5 m.
- the aromatic polyamide is preferably a polyamide containing a metaphenylene isophthalamide polymer as a main component.
- the porous membrane is obtained by casting a polymer solution containing an aromatic polyamide and an amide-based solvent as a main component on a support, and casting the cast product with an amide containing a substance incompatible with the aromatic polyamide. It is preferably produced by immersing in a system coagulation liquid to cause microphase separation, followed by washing and heat treatment.
- the electrolyte of the electric double layer capacitor is preferably a non-aqueous electrolyte, and the non-aqueous electrolyte is preferably an electrolyte in which an ammonium salt is dissolved. It preferably contains at least one asymmetric ammonium salt as a monium salt.
- the solvent of the non-aqueous electrolyte contains a non-aqueous solvent having a relative dielectric constant of 10 or more, preferably 80% by weight or more. The solvent is more preferably used.
- the non-aqueous electrolyte of the electric double layer capacitor may be an electrolyte containing an ionic liquid in an amount of 10% by weight or more.
- the present invention also encompasses the invention of an electric double layer capacitor using the above-described separator.
- the aromatic polyamide of the present invention is a polymer obtained by polycondensation of an aromatic diamine and an aromatic dicarboxylic acid halide.
- aromatic diamine include m-phenylenediamine, P-phenylenediamine, 1,4-diaminonaphthalene, 1,5-diaminonaphthalene, 1,8-diaminonaphthalene, and 2,6.
- aromatic dicarboxylic acid halide examples include phthalic acid, isophthalic acid, terephthalic acid, 1,6-naphthalenedicarboxylic acid, 1,7-naphthalenedicarboxylic acid, 2,6-naphthalenedicarboxylic acid, and 2,7-naphthalenedicarboxylic acid And dicarboxylic acid dihalides such as 3,4'-biphenyldicarboxylic acid and 4,4'-biphenyldicarboxylic acid. These diamines and dicarboxylic acid halides may be used alone or in combination of two or more.
- the aromatic polyamide used in the present invention is preferably an aromatic diamine such as metaphenylenediamine, paraphenylenediamine, or 3,4′-diaminodiphenyl ether from the viewpoint of physical properties and cost of the obtained porous membrane. It is preferable to use isohalic acid dihalide and terephthalic acid dihalide as the aromatic dicarbonic halide. More preferably, polymetaphenylene isophthalamide obtained by polycondensation of metaphenylenediamine and isophthalic acid dihalide is exemplified.
- the aromatic polyamide described above hexanediamine, decanediamine, dodecanediamine, ethylenediamine, aliphatic diamines such as hexamethylenediamine, or ethylenedicarboxylic acid, dicarboxylic acid dihalide such as hexamethylenedicarboxylic acid, It may be copolymerized in a proportion of 20 mol% or less based on the repeating unit of the polymer.
- the aromatic polyamide in the present invention when dissolved in N-methyl-2-pyrrolidone, has a logarithmic viscosity represented by the following formula (1) of 0.8 to 2.5 dlZg, preferably 1.0 to 2.2 dlZg.
- Preferred are polymers in the range. If the logarithmic viscosity is lower than 0.SdlZg, sufficient mechanical strength cannot be obtained, and if the logarithmic viscosity exceeds 2.5 dlZg, it becomes difficult to obtain a stable polymer solution, and a uniform porous membrane cannot be obtained. Not preferred.
- T Flow time of a solution prepared by dissolving 0.5 g of aromatic polyamide in 100 mL of ⁇ -methyl-2-pyrrolidone at 30 ° C by capillary viscometer
- Flow time of TO N-methyl-2-pyrrolidone at 30 ° C with capillary viscometer
- the aromatic polyamide porous membrane of the present invention may be prepared by any method.
- a polymer solution obtained by dissolving the above-mentioned aromatic polyamide in an amide-based solvent is cast on a support, and the cast product is subjected to amide-based coagulation containing a substance incompatible with the aromatic polyamide.
- the method of obtaining a porous membrane by immersing in a liquid to cause microphase separation, followed by washing and heat treatment has excellent controllability of the membrane structure and the productivity of the porous membrane of the present invention is excellent. It is preferable because a film can be formed.
- amide solvent used examples include polar amide solvents containing an amide group such as N-methyl-1-pyrrolidone, N, N-dimethylacetamide, and N, N-dimethylformamide.
- Examples of the support on which the polymer solution is cast include a glass substrate, a steel belt, a drum, and a polymer film such as polypropylene and polyethylene terephthalate. In consideration of productivity, it is preferable to use a polymer film. These polymer films may be subjected to release treatment of silicon or the like, corona discharge treatment, or the like.
- amide solvent used for the amide-based coagulation solution include N-methyl-2-pyrrolidone, N, N-dimethylacetamide, and N, N-dimethylformamide. These may be used in combination of two or more.
- substance incompatible with the aromatic polyamide include water, lower alcohols and lower ethers. These may be used in combination of two or more. Among them, the use of water alone is advantageous from the viewpoint of membrane characteristics and economical efficiency of the obtained porous membrane.
- the concentration of the amide solvent (for example, when 100% of N-methyl-2-pyrrolidone is used) in the amide-based coagulation liquid is, for example, in the case of a mixed solution with water, the concentration of the amide solvent is 40 a wt% to 80 wt%, more preferably 50 by weight% to 70 weight ⁇ 1 ⁇ 2, more preferably from 55 wt 1 1 ⁇ 2 ⁇ 70 wt%.
- Amide solvent When the concentration is less than 40% by weight, the mechanical strength of the obtained porous membrane is low, which is not preferable. When the concentration exceeds 80% by weight, it takes time to become a self-supporting porous film. Therefore, it is not preferable from the viewpoint of productivity.
- the solidified porous cast is then transferred to a washing step, where it is washed with water.
- the washed porous cast is then subjected to a heat treatment to dry the water, whereby the porous membrane of the present invention can be obtained. It is also possible to control the pore structure of the porous membrane by stretching the porous membrane simultaneously with the heat treatment.
- the film thickness of the aromatic polyamide multi-layer L film of the present invention is characterized in that it is in the range of 5 to 50 im. If the film thickness is less than 5 m, it is not preferable because it is difficult to secure electronic insulating properties and the mechanical strength becomes low, and handling becomes difficult. When the film thickness is 50 j ⁇ m or more, it is advantageous in terms of mechanical strength, but it is not preferable because not only the volume energy density of the capacitor is lowered but also the ion conductivity between the separators is lowered.
- the preferred range of the film thickness is 8 to 40 im, more preferably 10 to 30 jUm.
- the porosity of the aromatic polyamide polysaccharide L film of the present invention is characteristically in the range of 30 to 80%.
- the porosity indicates the ratio of the porosity in the porous body, and can be calculated by the following equation (2).
- the porosity is less than 30%, the electrolyte retention will be low, and the internal resistance of the capacitor will increase, which is not preferable. If the porosity exceeds 80%, the mechanical strength of the porous membrane will be poor. This is not preferred because internal short-circuiting is more likely to occur as well as handling becomes difficult.
- a more preferable range of the porosity is 40 to 75 ° / o, and further preferably 50 to 70%.
- the air permeability is a value measured according to JIS P8117.
- the air permeability of the aromatic polyamide porous film is 5 to 300 seconds Z1 ooir ⁇ 'of in 2 ranges der Rukoto features.
- the air permeability is larger than 100 mL 'in 2 for 300 seconds, a porous continuous structure is not sufficient, which is a factor that increases the internal resistance of the capacitor.
- the air permeability is less than 5 seconds ZIOOmL'in 2 , the self-discharge characteristics of the capacitor deteriorate, which is not preferable.
- the more preferable range of the air permeability is 10 to 200 seconds 1 OOml_-in 2 , more preferably 15 to 150 seconds / ⁇ OOmL 'in 2 .
- the puncture strength per unit film thickness of the aromatic polyamide porous film of the present invention is characterized by being 50 mN nom or more.
- the piercing strength is a property used for evaluating the separator as an index indicating the short-circuit prevention strength of the separator of the lithium ion secondary battery.In the present invention, the value measured under the following conditions is used as the unit film. Puncture per thickness and strength.
- the average internal pore diameter of the aromatic polyamide porous membrane of the present invention is preferably 0.01 to 5 m.
- the pore diameter of the porous membrane can be defined by various methods. In the present invention, a value calculated by image processing of a cross-sectional photograph by SEM observation is defined as an internal average pore diameter. The detailed measuring method will be described later. If the average pore diameter is less than 0.01 m, the ionic conductivity will decrease.Preferably, if the average pore diameter exceeds 5 m, an internal short circuit will occur when activated carbon or conductive agent used for the capacitor electrode falls off. Not desirable, because the probability of raising it rises.
- the more preferable range of the average pore diameter is from 0.003 to 3 m, more preferably from 0.05 to 2 im.
- the electric double layer capacitor of the present invention can be manufactured in the same manner as the conventional electric double layer capacitor, except that the aromatic polyamide porous film described above is used as a separator of the polarizable electrode.
- Some electric double layer capacitors use an aqueous electrolyte solution or a non-aqueous electrolyte solution.
- the aromatic polyamide porous membrane of the present invention can be applied to any electric double layer capacitor.
- the aromatic polyamide porous membrane of the present invention is a non-aqueous electrolyte. More preferably, the present invention is applied to an electric double-layer capacitor using the same.
- Non-aqueous electrolytes include, but are not particularly limited to, those commonly used for electric double layer capacitors.
- the electrolyte include a quaternary ammonium ion and a quaternary phosphonium ion whose cation components are, specifically, tetramethylammonium ion (Me4N +), tetraethylammonium ion (Et4N +), and ethyltrimethyl ion.
- Ammonia ion (Me3EtN +), getyldimethylammonium ion (Me 2Et2N +), triethylmethylammonium ion (Et3MeN +), tetrapropylammonium ion (Pr4N +), tetrabutylammonium ion (Bu4N + ;), Tributylmethylammonium ion (MeBu3N +), tetramethylphosphonium ion (Me4P +), tetraethylphosphonium ion (Et4P +), tetrapropylphosphonium ion (Pr4P +), tetra Butylphosphonium ion (Bu4P +).
- anion component examples include perfluorophosphate ion (BF4-) and hexafluorophosphate (PF6-). These salts composed of a cation component and an anion component may be used alone or in combination of two or more.
- ammonium salts are particularly preferred in terms of electrochemical stability and solubility in non-aqueous solvents, and more preferred are asymmetric ammonium salts such as triethylmethylammonium ion.
- the non-aqueous solvent in which these electrolytes are dissolved is preferably a solvent having a relative dielectric constant of 10 or more.
- propylene carbonate is used in addition to ethylene carbonate, butyl carbonate, dimethyl carbonate, vinylene carbonate, and the like. , 1,2-dimethoxyethane, 1,2-diethoxytan, monobutyrolactone, sulfolane, acetonitrile and the like. These may be used alone or as a mixture of two or more. It is also possible to add a solvent having a low relative dielectric constant as an additive, but in this case, it is preferable to mix the solvent having a relative dielectric constant of 10 or more so as to be 80% by weight or more.
- an ionic liquid as the electrolyte and / or the electrolyte as the non-aqueous electrolyte.
- the content of the ionic liquid must be 10% by weight or more. If the content of the ionic liquid is less than 10% by weight, the ionic conductivity of the electrolytic solution is undesirably low.
- Specific examples of the ionic liquid include cations such as alkylimidazolymion ions, alkylpyridinium ions, and alkylammonium ions.On the other hand, tetrafluoroborate ions and hexafluorofluorocarbon ions are used as counter anions.
- Phosphate and bistrifluoromethanesulfonimide are exemplified. These salts composed of the cation component and the anion component may be used alone or in combination of two or more.
- an ionic liquid When an ionic liquid is used as an electrolyte, it can be dissolved in the above-mentioned non-aqueous solvent to form an electrolyte.
- a 10,000 ⁇ magnification cross-section photograph observed with a scanning electron microscope with a resolution of 4 to 7 nm was developed at 150 ⁇ 200 mm in width and 2 million pixels using a scanner with a resolution of 30000 mm 2 and a diameter of 0,0 ⁇ ⁇ m
- the number of pixels was calculated for each of the above holes, and the total was divided by the number of holes to obtain an average hole area.
- the diameter when this was assumed to be a perfect circle was defined as the average hole diameter.
- a 1.5 M triethylmethylammonium tetrafluoroborate propylene carbonate solution was used as an electrolyte, and the evaluation was performed using a cell using a SUS electrode.
- the polymer used in this example was all poly (metaphenylene isophthalamide) (Conex J manufactured by Teijin Techno Products Limited), and its logarithmic viscosity (IV) was NMP (N— Methylpyrrolidone) as a solvent and a polymer concentration of 0.5 gZdL and a temperature of 30 ° C were 1.4.
- the true density of this polymer was 1.335 gZcm 3 .
- Conex polymer here.
- a polarizable electrode consisting of activated carbon (specific surface area: 1,200 mVg), conductive ffij agent (Ketchin black), and binder (polytetrafluoroethylene) is formed on a 20-m-thick aluminum foil, and a sheet-like electrode is formed. It was created. On both sides of the porous membrane obtained in (1), two sheet electrodes were sandwiched so that the polarizable electrode and the porous membrane were in close contact with each other, and water was removed at a temperature of 270 ° C.
- the polarizable electrode and the porous film were impregnated with a propylene carbonate solution of 1.5 M triethyl methylammonium tetrafluoroborate, which is an electrolytic solution, to produce a coin-type capacitor.
- a propylene carbonate solution of 1.5 M triethyl methylammonium tetrafluoroborate which is an electrolytic solution
- a porous film was formed under the same manufacturing conditions as in Example 1 except that the coating thickness of the dope was set to 100 / m. Table 1 shows the physical properties of the obtained porous membrane. Further, a coin-type capacitor was prepared in the same manner as in Example 1, and the capacity thereof was measured to be 1.2 FZcm 2 .
- a porous film was prepared under the same manufacturing conditions as in Example 1 except that the concentration of the dope was set to 10% by weight and the coating thickness of the dope was set to 120 m.
- the obtained porous membrane was stretched twice in an atmosphere of 280 ° C. to obtain a stretched aromatic polyamide porous membrane.
- Table 1 shows the physical properties of the obtained porous membrane.
- a coin-type capacitor was prepared in the same manner as in Example 1, except that a mixed solution of 1-ethyl-3-methylimidazolymtetrafluoroborate and propylene carbonate (weight ratio 3: 7) was used as the electrolyte.
- the capacity of the obtained capacitor was 0.9 Fcm 2 . ⁇ table 1
- the separator for electric double layer capacitors which has both excellent heat resistance and mechanical strength, high ionic conductivity and electrolyte retention.
- the use of this separator makes it possible to remove water at high temperatures and to perform heat treatment at the same time as the polarizable electrode, greatly improving the productivity and suppressing the contamination of water.
- a durable electric double layer capacity can be obtained.
- the film since the film has excellent mechanical strength, the film thickness can be reduced, and an electric double layer capacitor having a low internal resistance and a high energy density can be obtained.
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Abstract
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JP5167069B2 (ja) * | 2008-10-31 | 2013-03-21 | 帝人株式会社 | 非水系二次電池 |
KR101377476B1 (ko) | 2011-12-23 | 2014-03-26 | 웅진케미칼 주식회사 | 이차전지용 메타아라미드 다공성 막의 제조방법 및 그로부터 제조되는 다공성 막 |
US10044017B2 (en) | 2012-01-13 | 2018-08-07 | Toray Industries, Inc. | Aromatic polyamide porous film, separator for battery, and battery |
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JP2000281657A (ja) * | 1999-03-29 | 2000-10-10 | Sanyo Chem Ind Ltd | N−置換環状アミジンの製造方法 |
WO2001019906A1 (en) * | 1999-09-13 | 2001-03-22 | Teijin Limited | Polymethaphenylene isophthalamide based polymer porous film, method for producing the same and separator for cell |
JP2001332307A (ja) * | 2000-03-15 | 2001-11-30 | Teijin Ltd | 電解液担持ポリマー膜、電池用セパレータ、それらを用いた二次電池及びその製造方法 |
WO2001093350A1 (fr) * | 2000-05-29 | 2001-12-06 | Mitsubishi Paper Mills Limited | Separateur pour dispositif electrochimique, procede de production de ce dernier et dispositif electrochimique |
JP2002326977A (ja) * | 2001-05-02 | 2002-11-15 | Mitsubishi Gas Chem Co Inc | 電解質及び非水電解液の製造方法 |
JP2003133180A (ja) * | 2001-10-23 | 2003-05-09 | Du Pont Teijin Advanced Paper Kk | 電気二重層コンデンサ |
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JP2000281657A (ja) * | 1999-03-29 | 2000-10-10 | Sanyo Chem Ind Ltd | N−置換環状アミジンの製造方法 |
WO2001019906A1 (en) * | 1999-09-13 | 2001-03-22 | Teijin Limited | Polymethaphenylene isophthalamide based polymer porous film, method for producing the same and separator for cell |
JP2001332307A (ja) * | 2000-03-15 | 2001-11-30 | Teijin Ltd | 電解液担持ポリマー膜、電池用セパレータ、それらを用いた二次電池及びその製造方法 |
WO2001093350A1 (fr) * | 2000-05-29 | 2001-12-06 | Mitsubishi Paper Mills Limited | Separateur pour dispositif electrochimique, procede de production de ce dernier et dispositif electrochimique |
JP2002326977A (ja) * | 2001-05-02 | 2002-11-15 | Mitsubishi Gas Chem Co Inc | 電解質及び非水電解液の製造方法 |
JP2003133180A (ja) * | 2001-10-23 | 2003-05-09 | Du Pont Teijin Advanced Paper Kk | 電気二重層コンデンサ |
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