CN111933937B - 能量储存装置 - Google Patents
能量储存装置 Download PDFInfo
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- CN111933937B CN111933937B CN202010333960.5A CN202010333960A CN111933937B CN 111933937 B CN111933937 B CN 111933937B CN 202010333960 A CN202010333960 A CN 202010333960A CN 111933937 B CN111933937 B CN 111933937B
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- energy storage
- storage device
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- 238000004146 energy storage Methods 0.000 title claims abstract description 47
- 229920001577 copolymer Polymers 0.000 claims abstract description 150
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- 238000002955 isolation Methods 0.000 claims abstract description 10
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- 239000007784 solid electrolyte Substances 0.000 claims abstract description 5
- 239000000178 monomer Substances 0.000 claims description 54
- -1 2- (2-oxiranylmethoxy) ethyl Chemical group 0.000 claims description 23
- 125000000524 functional group Chemical group 0.000 claims description 19
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 16
- 239000000203 mixture Substances 0.000 claims description 16
- 125000003277 amino group Chemical group 0.000 claims description 14
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 claims description 14
- BAPJBEWLBFYGME-UHFFFAOYSA-N Methyl acrylate Chemical compound COC(=O)C=C BAPJBEWLBFYGME-UHFFFAOYSA-N 0.000 claims description 12
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 claims description 12
- 239000002002 slurry Substances 0.000 claims description 12
- XOAAWQZATWQOTB-UHFFFAOYSA-N taurine Chemical compound NCCS(O)(=O)=O XOAAWQZATWQOTB-UHFFFAOYSA-N 0.000 claims description 12
- 125000003700 epoxy group Chemical group 0.000 claims description 11
- VVJKKWFAADXIJK-UHFFFAOYSA-N Allylamine Chemical compound NCC=C VVJKKWFAADXIJK-UHFFFAOYSA-N 0.000 claims description 10
- RRHGJUQNOFWUDK-UHFFFAOYSA-N Isoprene Chemical compound CC(=C)C=C RRHGJUQNOFWUDK-UHFFFAOYSA-N 0.000 claims description 10
- 238000000576 coating method Methods 0.000 claims description 10
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- 229920002554 vinyl polymer Polymers 0.000 claims description 10
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- 239000011248 coating agent Substances 0.000 claims description 9
- 125000002883 imidazolyl group Chemical group 0.000 claims description 9
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- IQPQWNKOIGAROB-UHFFFAOYSA-N isocyanate group Chemical group [N-]=C=O IQPQWNKOIGAROB-UHFFFAOYSA-N 0.000 claims description 8
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- 125000001797 benzyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C([H])([H])* 0.000 claims description 7
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 claims description 7
- WOBHKFSMXKNTIM-UHFFFAOYSA-N Hydroxyethyl methacrylate Chemical compound CC(=C)C(=O)OCCO WOBHKFSMXKNTIM-UHFFFAOYSA-N 0.000 claims description 6
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- 125000004417 unsaturated alkyl group Chemical group 0.000 claims description 6
- WHNWPMSKXPGLAX-UHFFFAOYSA-N N-Vinyl-2-pyrrolidone Chemical compound C=CN1CCCC1=O WHNWPMSKXPGLAX-UHFFFAOYSA-N 0.000 claims description 5
- INLLPKCGLOXCIV-UHFFFAOYSA-N bromoethene Chemical compound BrC=C INLLPKCGLOXCIV-UHFFFAOYSA-N 0.000 claims description 5
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- 238000004132 cross linking Methods 0.000 claims description 4
- 238000009472 formulation Methods 0.000 claims description 4
- VOZRXNHHFUQHIL-UHFFFAOYSA-N glycidyl methacrylate Chemical compound CC(=C)C(=O)OCC1CO1 VOZRXNHHFUQHIL-UHFFFAOYSA-N 0.000 claims description 4
- 230000004048 modification Effects 0.000 claims description 4
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- CQEYYJKEWSMYFG-UHFFFAOYSA-N butyl acrylate Chemical compound CCCCOC(=O)C=C CQEYYJKEWSMYFG-UHFFFAOYSA-N 0.000 claims description 3
- KGIGUEBEKRSTEW-UHFFFAOYSA-N 2-vinylpyridine Chemical compound C=CC1=CC=CC=N1 KGIGUEBEKRSTEW-UHFFFAOYSA-N 0.000 claims description 2
- VVQNEPGJFQJSBK-UHFFFAOYSA-N Methyl methacrylate Chemical compound COC(=O)C(C)=C VVQNEPGJFQJSBK-UHFFFAOYSA-N 0.000 claims description 2
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- 125000003368 amide group Chemical group 0.000 claims description 2
- 229910052799 carbon Inorganic materials 0.000 claims description 2
- 125000002843 carboxylic acid group Chemical group 0.000 claims description 2
- 239000012948 isocyanate Substances 0.000 claims description 2
- 150000002513 isocyanates Chemical class 0.000 claims description 2
- RPQRDASANLAFCM-UHFFFAOYSA-N oxiran-2-ylmethyl prop-2-enoate Chemical compound C=CC(=O)OCC1CO1 RPQRDASANLAFCM-UHFFFAOYSA-N 0.000 claims description 2
- 229920006395 saturated elastomer Polymers 0.000 claims description 2
- 150000008053 sultones Chemical class 0.000 claims description 2
- XAYDWGMOPRHLEP-UHFFFAOYSA-N 6-ethenyl-7-oxabicyclo[4.1.0]heptane Chemical compound C1CCCC2OC21C=C XAYDWGMOPRHLEP-UHFFFAOYSA-N 0.000 claims 1
- DXPPIEDUBFUSEZ-UHFFFAOYSA-N 6-methylheptyl prop-2-enoate Chemical compound CC(C)CCCCCOC(=O)C=C DXPPIEDUBFUSEZ-UHFFFAOYSA-N 0.000 claims 1
- IEPRKVQEAMIZSS-UHFFFAOYSA-N Di-Et ester-Fumaric acid Natural products CCOC(=O)C=CC(=O)OCC IEPRKVQEAMIZSS-UHFFFAOYSA-N 0.000 claims 1
- IEPRKVQEAMIZSS-WAYWQWQTSA-N Diethyl maleate Chemical compound CCOC(=O)\C=C/C(=O)OCC IEPRKVQEAMIZSS-WAYWQWQTSA-N 0.000 claims 1
- 239000011884 anode binding agent Substances 0.000 claims 1
- 239000003013 cathode binding agent Substances 0.000 claims 1
- JBSLOWBPDRZSMB-FPLPWBNLSA-N dibutyl (z)-but-2-enedioate Chemical compound CCCCOC(=O)\C=C/C(=O)OCCCC JBSLOWBPDRZSMB-FPLPWBNLSA-N 0.000 claims 1
- OGVXYCDTRMDYOG-UHFFFAOYSA-N dibutyl 2-methylidenebutanedioate Chemical compound CCCCOC(=O)CC(=C)C(=O)OCCCC OGVXYCDTRMDYOG-UHFFFAOYSA-N 0.000 claims 1
- LDCRTTXIJACKKU-ARJAWSKDSA-N dimethyl maleate Chemical compound COC(=O)\C=C/C(=O)OC LDCRTTXIJACKKU-ARJAWSKDSA-N 0.000 claims 1
- UYMKPFRHYYNDTL-UHFFFAOYSA-N ethenamine Chemical compound NC=C UYMKPFRHYYNDTL-UHFFFAOYSA-N 0.000 claims 1
- 239000000853 adhesive Substances 0.000 abstract description 13
- 230000001070 adhesive effect Effects 0.000 abstract description 13
- 238000006116 polymerization reaction Methods 0.000 abstract description 5
- 230000002035 prolonged effect Effects 0.000 abstract description 4
- 230000000052 comparative effect Effects 0.000 description 43
- 238000006243 chemical reaction Methods 0.000 description 35
- 239000002033 PVDF binder Substances 0.000 description 28
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 27
- 238000002360 preparation method Methods 0.000 description 27
- 238000012360 testing method Methods 0.000 description 27
- 238000010438 heat treatment Methods 0.000 description 22
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 17
- 229910001416 lithium ion Inorganic materials 0.000 description 17
- VZSRBBMJRBPUNF-UHFFFAOYSA-N 2-(2,3-dihydro-1H-inden-2-ylamino)-N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]pyrimidine-5-carboxamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C(=O)NCCC(N1CC2=C(CC1)NN=N2)=O VZSRBBMJRBPUNF-UHFFFAOYSA-N 0.000 description 14
- 239000004743 Polypropylene Substances 0.000 description 14
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 14
- 229920001155 polypropylene Polymers 0.000 description 14
- 229910000572 Lithium Nickel Cobalt Manganese Oxide (NCM) Inorganic materials 0.000 description 13
- FBDMTTNVIIVBKI-UHFFFAOYSA-N [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] Chemical compound [O-2].[Mn+2].[Co+2].[Ni+2].[Li+] FBDMTTNVIIVBKI-UHFFFAOYSA-N 0.000 description 13
- 239000011888 foil Substances 0.000 description 13
- 239000007787 solid Substances 0.000 description 12
- 238000003756 stirring Methods 0.000 description 12
- 239000003999 initiator Substances 0.000 description 11
- 238000005096 rolling process Methods 0.000 description 11
- CERQOIWHTDAKMF-UHFFFAOYSA-M Methacrylate Chemical compound CC(=C)C([O-])=O CERQOIWHTDAKMF-UHFFFAOYSA-M 0.000 description 10
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- 229910052782 aluminium Inorganic materials 0.000 description 10
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 10
- 239000011230 binding agent Substances 0.000 description 10
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- LLLWMXQKXWIRDZ-UHFFFAOYSA-N 1-ethenylpyrrolidin-2-one Chemical compound C=CN1CCCC1=O.C=CN1CCCC1=O LLLWMXQKXWIRDZ-UHFFFAOYSA-N 0.000 description 8
- 238000007599 discharging Methods 0.000 description 8
- 125000004185 ester group Chemical group 0.000 description 8
- 229910052744 lithium Inorganic materials 0.000 description 8
- VGYDTVNNDKLMHX-UHFFFAOYSA-N lithium;manganese;nickel;oxocobalt Chemical compound [Li].[Mn].[Ni].[Co]=O VGYDTVNNDKLMHX-UHFFFAOYSA-N 0.000 description 8
- IQSHMXAZFHORGY-UHFFFAOYSA-N methyl prop-2-enoate;2-methylprop-2-enoic acid Chemical compound COC(=O)C=C.CC(=C)C(O)=O IQSHMXAZFHORGY-UHFFFAOYSA-N 0.000 description 8
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 7
- QABZOJKEJLITJL-UHFFFAOYSA-N but-3-enoic acid;ethenyl acetate Chemical compound CC(=O)OC=C.OC(=O)CC=C QABZOJKEJLITJL-UHFFFAOYSA-N 0.000 description 7
- 239000011889 copper foil Substances 0.000 description 7
- 239000002904 solvent Substances 0.000 description 7
- HMUNWXXNJPVALC-UHFFFAOYSA-N 1-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)C(CN1CC2=C(CC1)NN=N2)=O HMUNWXXNJPVALC-UHFFFAOYSA-N 0.000 description 6
- LDXJRKWFNNFDSA-UHFFFAOYSA-N 2-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-1-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]ethanone Chemical compound C1CN(CC2=NNN=C21)CC(=O)N3CCN(CC3)C4=CN=C(N=C4)NCC5=CC(=CC=C5)OC(F)(F)F LDXJRKWFNNFDSA-UHFFFAOYSA-N 0.000 description 6
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 6
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- 238000005119 centrifugation Methods 0.000 description 6
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- WZFUQSJFWNHZHM-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]piperazin-1-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)N1CCN(CC1)CC(=O)N1CC2=C(CC1)NN=N2 WZFUQSJFWNHZHM-UHFFFAOYSA-N 0.000 description 5
- KZPMXWBRKHQGQJ-UHFFFAOYSA-N 2-methyl-4-(oxiran-2-yl)but-2-enoic acid oxiran-2-ylmethyl 2-methylprop-2-enoate Chemical compound O1C(CC=C(C(=O)O)C)C1.C(C(=C)C)(=O)OCC1CO1 KZPMXWBRKHQGQJ-UHFFFAOYSA-N 0.000 description 5
- YLZOPXRUQYQQID-UHFFFAOYSA-N 3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)-1-[4-[2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidin-5-yl]piperazin-1-yl]propan-1-one Chemical compound N1N=NC=2CN(CCC=21)CCC(=O)N1CCN(CC1)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F YLZOPXRUQYQQID-UHFFFAOYSA-N 0.000 description 5
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- ZRPAUEVGEGEPFQ-UHFFFAOYSA-N 2-[4-[2-(2,3-dihydro-1H-inden-2-ylamino)pyrimidin-5-yl]pyrazol-1-yl]-1-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)ethanone Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C=1C=NN(C=1)CC(=O)N1CC2=C(CC1)NN=N2 ZRPAUEVGEGEPFQ-UHFFFAOYSA-N 0.000 description 3
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Abstract
一种能量储存装置,包括:两个电极;以及隔离层,其设置于该两个电极的间;该两个电极及该隔离层中的至少一个包含共聚高分子,该共聚高分子作为该能量储存装置的非水性粘合剂及/或固态电解质,用于电极或隔离层中,且该共聚高分子是丙烯腈与乙酸乙烯酯经聚合反应后所形成的共聚物或其衍生物。借此,可使应用该共聚高分子的能量储存装置具有较佳的充放电性质,可有效地延长能量储存装置的效率及寿命。
Description
技术领域
本发明涉及一种能量储存装置,特别涉及一种能量储存装置,其两个电极及隔离层中的至少一个包含共聚高分子,且该共聚高分子是丙烯腈与乙酸乙烯酯经聚合反应后所形成的共聚物或其衍生物。
背景技术
能量储存装置被广泛应用于各种电子产品中。能量储存装置中所使用的共聚高分子的物理及化学特性,对于能量储存装置的充放电效能具有一定程度的影响。因此,如何修饰该共聚高分子的化学结构,借此改善能量储存装置的充放电效能是本领域技术人员所努力的目标。
US 8993157B2揭示了一种电化学电池,其中,该电化学电池的阳极所使用的共聚高分子(PVDF-g-PAN)将丙烯腈基团接枝到由聚偏二氟乙烯(polyvinylidene difluoride,PVDF)所构成的主链上。
现有技术的能量储存装置中所使用的共聚高分子在改善能量储存装置的充放电效能方面,仍有进步的空间。
发明内容
本发明的目的在于,提供一种新颖的能量储存装置,其具有良好的充放电效能和优异的加工特性。
为达上述目的及其他目的,本发明提供一种能量储存装置,包括:
阳极及阴极;以及
隔离层,其设置于该阳极及该阴极之间;
其中,该阳极、阴极及隔离层中的至少一个包含共聚高分子,该共聚高分子作为该能量储存装置的水性或非水性粘合剂及/或电解质,其粘合剂适用于锂电池阴极、阳极或隔离层非水系的涂布制程,而前述的电解质包含胶态与固态,且该共聚高分子是丙烯腈与含有导离子基团的单体及/或含有乙烯基的单体经聚合反应后所形成的共聚物或其衍生物。
于本发明的一实施例中,该能量储存装置可为电池、电容或燃料电池。
于本发明的一实施例中,该共聚高分子含有如下列所示的结构:
其中:
GI衍生自丙烯腈或含有腈基的单体;
GII衍生自含有导离子基团的极性单体,其中R2包含下列官能基其中至少一种或其组合:酰胺(amide)、胺基(amino group)、吡咯烷酮基(pyrrolidone group)、醚基(ethergroup)、咪唑基(imidazole group)、铵基(Ammonium group,R-NH3 +、(R)2-NH2 +、(R)3-NH+、(R)4-N+)、羧基(carboxy group),其羧基包含丙烯酸(acrylic acid)、甲基丙烯酸(methacrylic acid)、马来酸(maleic acid)、亚甲基丁二酸(itaconic acid)等,含硫化物的酸基,如:磺酸基(sulfonic acid group,-SO3H)、硫酸基(sulfuric group),含磷化物的酸基,如:磷酸基(phosphoric acid group,-PO3H3),以及上述酸基所衍生的酯基(estergroup)或上述酸基、吡咯烷酮基以及咪唑基等四级铵、四级磷所衍生的盐基(salt group);
GIII衍生自含有反应性官能基的单体,其中R3可包含下列官能基中一种或其组合:具有C1~C30饱和与不饱和烷基(Alkyl group)的酯基(ester group)、羟基(Hydroxygroup)、环氧基(Epoxy group)、异氰酸酯基(isocyanate group)、胺基(amino group);
GIV衍生自含有乙烯基的单体(olefinic monomer),其中R4可包含下列官能基中一种或其组合:C1~C30饱和与不饱和的烷基(Alkyl group)、苯基(Phenyl group)、苯甲基(benzyl group);
其中R1为H或CH3;
其中,该共聚高分子的重复单元的数量符合下列条件:
于本发明的一实施例中,该共聚高分子中:
GI衍生自丙烯腈或含有腈基的单体
GII衍生自含有导离子基团的极性单体,其可包含自下列化合物中的至少一种或其组合:N-乙烯基吡咯烷酮(n-vinylpyrrolidone)、丙烯酰胺(Acrylamide)、甲基丙烯酰胺(methacrylamide)、二甲基丙烯酰胺(N,N-dimethyl acrylamide)、二乙基丙烯酰胺(N,N-diethyl acrylamide)、丙烯酰吗啉(Acryloyl morpholine)、丙烯酸(Acrylic acid)、甲基丙烯酸(Methacrylic acid)、乙酸乙烯酯(vinyl acetate)、聚(乙二醇)甲基丙烯酸酯(Poly(ethylene glycol)methacrylate)、磺酸苯乙烯(polystyrene sulfonate);
GIII衍生自含有反应性官能基的单体,其可包含自下列化合物中的一种或其组合:甲基丙烯酸缩水甘油酯(Glycidyl methacrylate)、丙烯酸缩水甘油酯(Glycidylacrylate)、乙烯基环氧环己烷(Vinyl epoxy cyclohexane)、甲基丙烯酸2-(2-环氧乙烷基甲氧基)乙酯(2-(2-Oxiranylmethoxy)ethyl methacrylate)、甲基丙烯酸羟乙酯(2-Hydroxyethyl methacrylate)、烯丙基胺(Allylamine)、乙烯胺(vinylamine);
GIV衍生自含有乙烯基的单体(olefinic monomer),其可包含自下列化合物中的一种或其组合:丙烯酸异辛酯(2-Ethylhexyl acrylate)、丙烯酸丁酯(n-Butyl acrylate)、丙烯酸异丁酯(isobutyl acrylate)、丙烯酸甲酯(Methyl acrylate)、氯乙烯(Vinylchloride)、二氯乙烯(vinylidene chloride)、溴乙烯(vinyl bromide)、亚甲基丁二酸二丁酯(Dibutyl Itaconate)、马来酸二甲酯(Dimethyl maleate)、、马来酸二乙酯(Diethylmaleate)、马来酸二丁酯(Dibutyl maleate)、苯乙烯(Styrene)、甲基丙烯酸甲酯(Methylmethacrylate)、丁二烯(1,3-Butadiene)、异戊二烯(Isoprene)。
为达上述目的及其他目的,本发明也提供一种能量储存装置,包括:
两个电极;以及
隔离层,其设置于该两个电极之间;
其中,该两个电极及该隔离层中的至少一个包含共聚高分子,该共聚高分子含有如下列所示的结构:
其中:
GI衍生自丙烯腈;
GII衍生自乙酸乙烯酯(vinyl acetate);
GIII衍生自含有反应性官能基的单体,其中R3包含下列官能基中一种或其组合:具有C1~C30饱和与不饱和烷基(Alkyl group)的酯基(Ester group)、羟基(Hydroxy group)、环氧基(Epoxy group)、异氰酸酯基(isocyanate group)、胺基(amino group);
GIV衍生自含有乙烯基的单体(olefinic monomer),其中R4包含下列官能基中一种或其组合:酰胺基(amide group)、吡咯烷酮基(pyrrolidone group)、C1~C30饱和与不饱和的烷基(Alkyl group)、苯基(Phenyl group)、苯甲基(benzyl group);
其中R1为H或CH3;
其中,该共聚高分子的重复单元的数量符合下列条件:
于本发明的一实施例中,该共聚高分子中:
GIII衍生自含有反应性官能基的单体,其中该含有反应性官能基的单体选自由丙烯酸甲酯(methyl acrylate)、甲基丙烯酸缩水甘油酯(Glycidyl methacrylate)、丙烯酸缩水甘油酯(Glycidyl acrylate)、乙烯基环氧环己烷(Vinyl epoxy cyclohexane)、甲基丙烯酸2-(2-环氧乙烷基甲氧基)乙酯(2-(2-Oxiranylmethoxy)ethyl methacrylate)、甲基丙烯酸羟乙酯(2-Hydroxyethyl methacrylate)、烯丙基胺(Allylamine)及乙烯胺(vinylamine)所组成的组;
GIV衍生自含有乙烯基的单体(olefinic monomer),其中该含有乙烯基的单体选自由丙烯酰胺(Acrylamide)、N-乙烯基吡咯烷酮(N-Vinylpyrrolidone)、N,N-二甲基丙烯酰胺(N,N-Dimethylacrylamide)、丙烯酸异辛酯(2-Ethylhexyl acrylate)、N-乙烯基吡咯烷酮(N-Vinylpyrrolidone)、氯乙烯(Vinyl chloride)、二氯乙烯(vinylidene chloride)、溴乙烯(vinyl bromide)、丙烯酸丁酯(n-Butyl acrylate)、丙烯酸异丁酯(isobutylacrylate)、亚甲基丁二酸二丁酯(Dibutyl Itaconate)、马来酸二甲酯(Dimethylmaleate)、马来酸二乙酯(Diethyl maleate)、马来酸二丁酯(Dibutyl maleate)、苯乙烯(Styrene)、丙烯酸甲酯(Methyl acrylate)、乙烯基吡啶(Vinyl pyridine)、甲基丙烯酸甲酯(Methyl methacrylate)、丁二烯(1,3-Butadiene)及异戊二烯(Isoprene)所组成的组。
于本发明的一实施例中,该能量储存装置是电池,且该两个电极包含:阳极及阴极。
于本发明的一实施例中,该共聚高分子进一步与含氨基(amino group)、异氰酸酯(isocyanate group)、羟基(Hydroxyl group)、羧酸基(Carboxylic group)、咪唑基(imidazole)的化合物反应,或与牛磺酸(Taurine)、磺内酯(1,3-Propanesultone)或其衍生物中的一种或其组合进行反应,以获得改质或交联。
本发明中的共聚高分子可经由自由基聚合、活性自由基聚合、乳化聚合或氧化还原聚合而制备而成。
举例来说,该共聚高分子中由含有环氧基的单体(例如:甲基丙烯酸缩水甘油酯)所衍生的重复单元中的环氧基团可进行开环反应,借此衔接一非离子、阳离子或阴离子基团以获得改质或交联,或可借由开环反应与另一共聚高分子形成交联结构。具体而言,该共聚高分子可进一步与例如:聚醚氨(polyether amine)、牛磺酸(Taurine)、聚醚二氨(polyether diamine)、咪唑(imidazole)或其衍生物进行反应以获得改质或交联,并可将经改质或交联的共聚高分子应用于本发明的能量储存装置。
于本发明的一实施例中,该能量储存装置的阳极含有活性物质、导电碳以及该共聚高分子,且该共聚高分子的含量占该阳极的0.01%~30%重量百分比。
于本发明的一实施例中,该共聚高分子的含量占该阴极的0.01%~30%重量百分比。
于本发明的一实施例中,该隔离层经由涂布浆料或配方所形成,其中,该共聚高分子的含量占该浆料或配方成分的0.1%~30%重量百分比。
于本发明的一实施例中,该共聚高分子与任一高分子混掺作为该能量储存装置的固态电解质,且该共聚高分子的含量占该固态电解质成分的0.1%~90%重量百分比。
本发明的能量储存装置具有较佳的充放电性质,借由应用特定的共聚高分子,可有效地延长该能量储存装置的效率及寿命,并同时拥有较佳的加工特性。
附图说明
图1是包含共聚高分子P(AN-GMA-NVP)的锂镍钴锰氧正极的粘着力测试结果。
图2是包含共聚高分子P(AN-GMA-MMA)的锂镍钴锰氧正极的粘着力测试结果。
图3是包含PVDF的锂镍钴锰氧正极的粘着力测试结果。
图4是实施例8-1的共聚高分子的DSC测试结果。
图5是实施例8-2的共聚高分子的DSC测试结果。
图6是实施例8-3的共聚高分子的DSC测试结果。
图7是实施例8-4的共聚高分子的DSC测试结果。
图8是实施例8-5的共聚高分子的DSC测试结果。
图9是比较例3-1的共聚高分子的DSC测试结果。
图10是比较例3-2的共聚高分子的DSC测试结果。
图11是比较例3-3的共聚高分子的DSC测试结果。
具体实施方式
为充分了解本发明的目的、特征及功效,借由下述具体的实施例,对本发明做一详细说明,说明如后:
本发明的能量储存装置中所应用的共聚高分子可为丙烯腈与含有导离子基团的单体及/或含有乙烯基的单体经聚合反应后所形成的共聚物或其衍生物。举例来说,该含有乙烯基的单体可为乙烯基吡咯烷酮、丙烯酸甲酯、聚(乙二醇)甲基丙烯酸酯、苯乙烯、甲基丙烯酸甲酯(压克力的单体)或乙烯基吡啶。此外,该共聚高分子可为丙烯腈与含有导离子基团的单体、含有乙烯基的单体及/或含有环氧基的单体经聚合反应后所形成的共聚物或其衍生物。该含有环氧基的单体可为甲基丙烯酸缩水甘油酯(Glycidyl methacrylate)、丙烯酸缩水甘油酯(Glycidyl acrylate)、乙烯基环氧环己烷(Vinyl epoxy cyclohexane)或甲基丙烯酸2-(2-环氧乙烷基甲氧基)乙酯(2-(2-Oxiranylmethoxy)ethylmethacrylate),且该共聚高分子可含有如下列所示的结构。
其中:
GI衍生自丙烯腈;
GII衍生自含有导离子基团的极性单体,其中R2包含下列官能基其中至少一种或其组合:酰胺(amide)、胺基(amino group)、吡咯烷酮基(pyrrolidone group)、醚基(ethergroup)、咪唑基(imidazole group)、铵基(Ammonium group,R-NH3 +、(R)2-NH2 +、(R)3-NH+、(R)4-N+)、羧基(carboxy group),其羧基包含丙烯酸(acrylic acid)、甲基丙烯酸(methacrylic acid)、马来酸(maleic acid)、亚甲基丁二酸(itaconic acid)等,含硫化物的酸基,如:磺酸基(sulfonic acid group,-SO3H)、硫酸基(sulfuric group),含磷化物的酸基,如:磷酸基(phosphoric acid group,-PO3H3),以及上述酸基所衍生的酯基(estergroup)或上述酸基、吡咯烷酮基以及咪唑基等四级铵、四级磷所衍生的盐基(salt group);
GIII衍生自含有反应性官能基的单体,其中R3包含下列官能基中一种或其组合:羟基(Hydroxy group)、环氧基(Epoxy group)、异氰酸酯基(isocyanate group)、胺基(aminogroup);
GIV衍生自含有乙烯基的单体(olefinic monomer),其中R4包含下列官能基中一种或其组合:C1~C30饱和与不饱和的烷基(Alkyl group)、苯基(Phenyl group)、苯甲基(benzyl group);
其中R1为H或CH3;
其中,该共聚高分子的重复单元的数量符合下列条件:
在本发明的一实施例中,重复单元的数量a可为100~50000;重复单元的数量b可为100~10000;重复单元的数量c可为100~10000;以及重复单元的数量d可为100~10000。
实施例1
实施例1-1:P(AN-NVP)的制备
将丙烯腈(2-propenenitrile)与N-乙烯基吡咯烷酮(N-Vinylpyrrolidone)以重量比9:1的比例搅拌混合,再加入适量偶氮二异丁醚盐酸盐作为起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得即为丙烯腈-吡咯烷酮共聚物。将此产物命名为P(AN-NVP)。
实施例1-1的合成物如式(IV)所示
a与b比例是9:1。
实施例1-2:P(AN-Am)的制备
将丙烯氰与甲基丙烯酰胺(methacrylamide)以重量比9:1的比例搅拌混合,再加入适量起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得即为丙烯腈甲基丙烯酸甲酯共聚物。将此产物命名为P(AN-Am)。
实施例1-2的合成物如式(V)所示
其中,R1是-NH2;
R’是-CH3;
a与b比例是9:1。
实施例1-3:P(AN-AA)的制备
将丙烯氰与丙烯酸(Acrylic acid)以重量比9:1的比例搅拌混合,再加入适量起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得即为丙烯腈-丙烯酸共聚物。将此产物命名为P(AN-AA)。
实施例1-3的合成物如式(VI)所示
其中,
a与b比例是9:1;
R1及R’是H。
实施例1-4:P(AN-GMA-NVP)的制备
将丙烯腈(2-propenenitrile)与甲基丙烯酸缩水甘油酯(Glycidylmethacrylate)以及N-乙烯基吡咯烷酮(N-Vinylpyrrolidone)以重量比9:1:1的比例搅拌混合,再加入适量偶氮二异丁醚盐酸盐作为起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得即为丙烯腈-甲基丙烯酸缩水甘油酯-吡咯烷酮共聚物。将此产物命名为P(AN-GMA-NVP)。
实施例1-4的合成物如式(VII)所示
a与b与c比例是9:1:1。
实施例1-5:P(AN-GMA-MMA)以聚醚氨改质共聚高分子的制备
将实施例1-4所合成的P(AN-GMA-MMA)3g溶于NMP 20ml中,并加入0.3g的聚醚氨(M1000,Huntsman),60℃下反应6小时即可得到聚醚氨改质的P(AN-GMA-MMA)。
实施例1-6:P(AN-GMA-MMA)以聚醚二氨改质交联高分子的制备
将实施例1-4所合成的P(AN-GMA-MMA)3g溶于NMP 20ml中,并加入0.3g的聚醚二氨(ED2003,Huntsman),60℃下反应6小时即可得到以聚醚二氨改质交联的P(AN-GMA-MMA)高分子。
实施例1-7:P(AN-GMA-MMA)以阴离子基团改质共聚高分子的制备
将实施例1-4所合成的P(AN-GMA-MMA)3g溶于NMP 20ml中,并加入0.1g的牛磺酸,60℃下反应6小时即可得到以阴离子基团改质交联的P(AN-GMA-MMA)高分子。
实施例2
实施例2-1:P(AN-ALi-PEGMA-VP)的制备
将丙烯腈(2-propenenitrile),甲基丙烯酸缩水甘油酯(Glycidylmethacrylate),聚(乙二醇)甲基丙烯酸酯(Polyethylene glycol methacrylate),N-乙烯基吡咯烷酮(N-Vinylpyrrolidone)以重量比9:1:0.5:0.5的比例搅拌混合,再加入适量起始剂。加热至60℃,持续反应12小时。反应12小时后,再加入1M的LiOH进入反应器中搅拌24小时,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得的丙烯腈共聚物,命名为P(AN-ALi-PEGMA-VP)。
实施例2-1的合成物如式(VIII)所示:
其中,R1是-CH3;
R’是Li;
R”是-CH3;
a、b、c与d比例是9:1:0.5:0.5。
实施例2-2:P(AN-GMA-PEGMA-MMA)的制备
将丙烯腈(2-propenenitrile),甲基丙烯酸缩水甘油酯(Glycidylmethacrylate),聚(乙二醇)甲基丙烯酸酯(Polyethylene glycol methacrylate),丙烯酸甲酯(methyl methacrylate)以重量比9:1:0.5:0.5的比例搅拌混合,再加入适量起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得的丙烯腈共聚物,命名为P(AN-GMA-PEGMA-MMA)。
实施例2-2的合成物如式(IX)所示
其中,R1是-CH3;
R’是-CH3;
R”是-CH3;
a、b、c与d比例是9:1:0.5:0.5。
实施例2-3:P(AN-Am-VP-SSt)的制备
将丙烯腈(2-propenenitrile),甲基丙烯酰胺(methacrylamide),N-乙烯基吡咯烷酮(N-Vinylpyrrolidone),磺酸苯乙烯(sulfonated styrene)以重量比9:1:0.5:0.5的比例搅拌混合,再加入适量起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得的丙烯腈共聚物,命名为P(AN-Am-VP-SSt)。
实施例2-3的合成物如式(X)所示
R’是-NH2;
其中,a、b、c与d比例是9:1:0.5:0.5。
实施例3
实施例3-1:P(AN-GMA-PEGMA-MMA-VP)的制备
将丙烯腈(2-propenenitrile),甲基丙烯酸缩水甘油酯(Glycidylmethacrylate),聚(乙二醇)甲基丙烯酸酯(Polyethylene glycol methacrylate),丙烯酸甲酯(methyl methacrylate),与N-乙烯基吡咯烷酮(N-Vinylpyrrolidone)以重量比9:0.15:0.15:1:1的比例搅拌混合,再加入适量起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得的丙烯腈共聚物,命名为P(AN-GMA-PEGMA-MMA-VP)。
实施例3-1的合成物如式(XI)所示
其中,R1是-CH3;
R’是_-CH3;
R”是-CH3;
a、b、c、d与e比例是9:0.15:0.15:1:1。
实施例3-2:P(AN-Mam-EG-VP-Im)的制备
将丙烯腈(2-propenenitrile),N,N-二甲基甲基丙烯酰胺(N,N-Dimethylmethacrylamide),聚(乙二醇)甲基丙烯酸酯(Polyethylene glycolmethacrylate),与N-乙烯基吡咯烷酮(N-Vinylpyrrolidone),1-乙烯基咪唑(1-Vinylimidazole)以重量比8.9:1:0.2:0.2:0.7的比例搅拌混合,再加入适量起始剂。加热至60℃,持续反应12小时。反应12小时后,将析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得的丙烯腈共聚物,命名为P(AN-Mam-EG-VP-Im)。
实施例3-2的合成物如式(XII)所示
其中,R1是-CH3;
R’是-N(CH3)2;
R”是-CH3;
a、b、c、d与e比例是8.9:1:0.2:0.2:0.7。
实施例4
实施例4-1,制备各别以实施例1-1~3-2的共聚高分子作为粘着剂的锂镍钴锰氧(Li(NiCoMn)O2)正极极片
将实施例1-1~3-2所制备的共聚高分子作为粘着剂,与商用碳粉(Super P),商用锂镍钴锰氧(Li(NiCoMn)O2,BASF)以重量比2.1:2.5:95.4的比例混合并以NMP作为溶剂,以旋转搅拌机(海裕)搅拌1小时。将搅拌完成的浆料以自动涂布机(elcometer,3570)涂布在铝箔上后,置入真空烘箱升温至100℃,加热24小时后取出,以碾压机滚压极片,即可得含有实施例1-1~3-2的共聚高分子的锂镍钴锰氧正极。
实施例4-2:含共聚高分子正极的拉力测试
将实施例4-1所制备正极试片,贴上3M胶带,以拉力机(ALGOL,JSV-HS1000)进行拉力测试。
图1是使用实施例1-1的P(AN-NVP)作为正极的粘着剂的正极拉力测试结果。图2是使用实施例1-2的P(AN-Am)作为正极的粘着剂的正极拉力测试结果。可以观察到实施例1-1与1-2,皆比PVDF有较优异的附着力。
实施例4-3:含共聚高分子正极的锂离子电池的充放电测试
将实施例4-1所制备的正极极片,分别以钮扣型电池形式组装。首先,将商用聚丙烯(Polypropylene,PP)膜作为隔离层置于上述锂镍钴锰氧(Li(NiCoMn)O2)正极与锂金属负极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含共聚高分子的正极锂离子半电池的充放电效能。电位设定范围为2.8~4.2V,充电电流值设定为0.1C,放电电流值设定为0.1C、0.5C、1C、3C、5C,结果如下表所示。
上述含有共聚高分子正极的锂离子半电池在不同电流值设定下,所得到的放电电容值,如表1~表8所示。由表1~8可观察在不同比例与共聚高分子的组成中,相较于PVDF作为电极接着剂,在不同充放电电流下皆具有较优异的充放电性能。
表1:含实施例1-1的共聚高分子的正极半电池在不同充放电流值下电容量
表2:含实施例1-2的共聚高分子的正极半电池在不同充放电流值下电容量
表3:含实施例1-3的共聚高分子的正极半电池在不同充放电流值下电容量
表4:含实施例1-4的共聚高分子的正极半电池在不同充放电流值下电容量
表5:含实施例1-5的共聚高分子的正极半电池在不同充放电流值下电容量
表6:含实施例1-6的共聚高分子的正极半电池在不同充放电流值下电容量
表7:含实施例1-7的共聚高分子的正极半电池在不同充放电流值下电容量
表8:含实施例2-1的共聚高分子的正极半电池在不同充放电流值下电容量
表9:含实施例2-2的共聚高分子的正极半电池在不同充放电流值下电容量
表10:含实施例2-3的共聚高分子的正极半电池在不同充放电流值下电容量
表11:含实施例3-1的共聚高分子的正极半电池在不同充放电流值下电容量
表12:含实施例3-2的共聚高分子的正极半电池在不同充放电流值下电容量
实施例5
实施例5-1,制备各别以实施例1-1~3-2的共聚高分子作为粘着剂的石墨负极极片
将实施例1-1~3-2所制备的共聚高分子作为粘着剂,与商用碳粉(Super P),商用石墨以重量比3.8:1.8:94.4的比例混合并以NMP作为溶剂,以旋转搅拌机(海裕)搅拌1小时。将搅拌完成的浆料以自动涂布机(elcometer,3570)涂布在铜箔上后,置入真空烘箱升温至100℃,加热24小时后取出,以碾压机滚压极片,即可得含有实施例1-1~3-2的共聚高分子的石墨负极极片。
实施例5-2:含共聚高分子负极的锂离子电池的充放电测试
将实施例5-1所制备的负极极片,分别以钮扣型电池形式组装。首先,将商用聚丙烯(Polypropylene,PP)膜作为隔离层置于上述石墨负极与锂金属正极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含共聚高分子的负极的锂离子半电池的充放电效能。电位设定范围为0.05~2V,充电电流值设定为0.1C,放电电流值设定为0.1C、0.5C、1C、3C、5C。
上述含有共聚高分子的锂离子半电池在不同电流值设定下,所得到的放电电容值,如表13、表14所示。依据表13与14结果可知,在实施例1-1与1-2共聚高分子皆可在负极测试中较PVDF有较佳的表现。
表13:含实施例1-1的共聚高分子负极半电池在不同充放电流值下的电容量
表14:含实施例1-2的共聚高分子负极半电池在不同充放电流值下的电容量
实施例6
实施例6-1,制备各别以实施例1-1的共聚高分子作为粘着剂的陶瓷涂布隔离层
将实施例1-1所制备的共聚高分子作为模离模涂布的粘着剂,将1-1所制备的共聚高分子溶于NMP中,后将氧化铝(Al2O3)粉末与1-1共聚高分子依8:2重量比例均匀分散于NMP溶液中,后涂布于模离膜上,利用80℃烘干即可得陶瓷涂布的隔离层。
将实施例6-1所制备的陶瓷涂布隔离层,分别以钮扣型电池形式组装。首先,将陶瓷涂布隔离层作为隔离层于锂镍钴锰氧(Li(NiCoMn)O2)正极与锂金属负极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含共聚高分子的锂离子半电池的充放电效能。电位设定范围为0.05~2V,充电电流值设定为0.1C,放电电流值设定为0.1C、0.5C、1C、3C、5C。
表15:含实施例6-1的陶瓷涂布的隔离层组成半电池在不同充放电流值下的电容量
综合上述实施例可了解,本发明的能量储存装置中所包含的共聚高分子可具有一种以上如式(A)所示的重复单元(例如:实施例2-3、3-2):
也可具有一种以上如式(B)所示的重复单元(例如:实施例2-2、3-1):
此外本发明的能量储存装置中所包含的共聚高分子也可具有上述式(A)及式(B)所示的重复单元的任意组合。
实施例7
实施例7-1将实施例1-1的共聚高分子与商用PVDF混掺作为粘着剂的锂镍钴锰氧(Li(NiCoMn)O2)正极极片
将PVDF、实施例1-1的P(AN-NVP)共聚高分子与商用Super P及商用锂镍钴锰氧(Li(NiCoMn)O2,BASF)以重量比1.05:1.05:2.5:95.4的比例混合并以NMP做溶剂,以旋转搅拌机(海裕)搅拌1小时。将搅拌完成的浆料以自动涂布机(elcometer,3570)涂布在铝箔上后,置入真空烘箱升温至100℃,加热24小时后取出,以碾压机滚压极片,即可得以PVDF与实施例1-1的P(AN-NVP)作为粘着剂的锂镍钴锰氧正极。
实施例7-2:将实施例7-1所制备的PVDF锂镍钴锰氧(Li(NiCoMn)O2)正极,分别以钮扣型电池形式组装。首先,将商用聚丙烯(Polypropylene,PP)膜作为隔离层置于上述锂镍钴锰氧(Li(NiCoMn)O2)正极与锂金属负极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含有Pristine PVDF的正极锂离子半电池的充放电效能。电位设定范围为2.8~4.2V,充电电流值设定为0.1C,放电电流值设定为0.1C、0.5C、1C、3C、5C。
表16:含实施例1-1的共聚高分子与PVDF混掺的正极半电池在不同充放电流值下电容量
比较例1:Pristine PVDF正极
比较例1-1:使用聚偏二氟乙烯(polyvinylidene difluoride,PVDF)作为为粘着剂的锂镍钴锰氧(Li(NiCoMn)O2)正极材料的制备
将PVDF与商用Super P及商用锂镍钴锰氧(Li(NiCoMn)O2,BASF)以重量比2.1:2.5:95.4的比例混合并以NMP做溶剂,以旋转搅拌机(海裕)搅拌1小时。将搅拌完成的浆料以自动涂布机(elcometer,3570)涂布在铝箔上后,置入真空烘箱升温至100℃,加热24小时后取出,以碾压机滚压极片,即可得以Pristine PVDF作为粘着剂的锂镍钴锰氧正极。
比较例1-2:将比较例1-1所制备PVDF的正极试片,贴上3M胶带,以拉力机(ALGOL,JSV-HS1000)进行拉力测试。
图3是使用比较例1-1的PVDF作为正极的粘着剂的正极拉力测试结果。
比较例1-3:将比较例1-1所制备的PVDF锂镍钴锰氧(Li(NiCoMn)O2)正极,分别以钮扣型电池形式组装。首先,将商用聚丙烯(Polypropylene,PP)膜作为隔离层置于上述锂镍钴锰氧(Li(NiCoMn)O2)正极与锂金属负极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含有Pristine PVDF的正极锂离子半电池的充放电效能。电位设定范围为2.8~4.2V,充电电流值设定为0.1C,放电电流值设定为0.1C、0.5C、1C、3C、5C。
比较例1-3的正极锂离子半电池在不同电流值设定下,所得到的放电电容值,如表17所示。
表17:
比较例2:PVDF(负极)
比较例2-1:使用PVDF作为粘着剂的石墨负极极片的制备
将PVDF与商用Super P及商用石墨以重量比2.1:2.5:95.4的比例混合并以NMP做溶剂,以旋转搅拌机(海裕)搅拌1小时。将搅拌完成的浆料以自动涂布机(elcometer,3570)涂布在铜箔上后,置入真空烘箱升温至100℃,加热24小时后取出,以碾压机滚压极片,即可得PVDF粘着剂的石墨负极。
比较例2-2:将比较例2-1所制备的PVDF石墨负极,分别以钮扣型电池形式组装。首先,将商用聚丙烯(Polypropylene,PP)膜作为隔离层置于上述锂镍钴锰氧(Li(NiCoMn)O2)正极与PVDF石墨负极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含PVDF粘着剂的负极锂离子半电池的充放电效能。电位设定范围为0.5~2V,充电电流值设定为0.1C,放电电流值设定为0.1C、0.5C、1C、3C、5C。
比较例2-2的负极锂离子电池在不同电流值设定下,所得到的放电电容值,如表18所示。
表18:
由图1~图3的结果可知,使用本发明的共聚高分子作为粘着剂,相较于比较例1的PVDF,可使浆料有较佳的粘着效果,此结果因本发明的共聚高分子具有由丙烯腈所衍生的重复单元所致。
由上述图1~图3及表1~表18的结果可知,使用实施例1-1~3-2的共聚高分子所制备的锂离子电池具有优异的充放电性质。
综合上述实施例及比较例的测试结果可理解,本发明的能量储存装置于阳极、阴极及隔离层中的至少一个包含共聚高分子,且该共聚高分子是丙烯腈与含有导离子基团的单体及/或含有乙烯基的单体经聚合反应后所形成的共聚物或其衍生物。借此,可使应用该共聚高分子的能量储存装置具有较佳的充放电性质,可有效地延长能量储存装置的效率及寿命。
实施例8
实施例8-1:P(AN-VAc)的制备
将反应单体丙烯腈(acrylonitrile)、乙酸乙烯酯(Vinyl acetate)以重量比70:30的比例搅拌混合,再加入适量偶氮二异丁腈(Azobisisobutyronitrile,AIBN)起始剂于二甲基亚砜(DMSO)中。加热至60℃,持续反应12小时。反应12小时后,将产物以甲醇析出,析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得的丙烯腈共聚物,命名为P(AN-VAc)。
实施例8-2:P(AN-VAc-MA)的制备
反应流程同上但将反应单体改为丙烯腈(acrylonitrile)、乙酸乙烯酯(Vinylacetate)、丙烯酸甲酯(methyl acrylate)以重量比80:10:10的比例搅拌混合。所得的丙烯腈共聚物,命名为P(AN-VAc-MA)。
实施例8-3:P(AN-VAc-MA-Am)的制备
反应流程同上但将反应单体改为丙烯腈(acrylonitrile)、乙酸乙烯酯(Vinylacetate)、丙烯酸甲酯(methyl acrylate)、丙烯酰胺(Acrylamide)以重量比76:(9.5):(9.5):5的比例搅拌混合。所得的丙烯腈共聚物,命名为P(AN-VAc-MA-Am)。
实施例8-4:P(AN-VAc-MA-NVP)的制备
反应流程同上但将反应单体改为丙烯腈(acrylonitrile)、乙酸乙烯酯(Vinylacetate)、丙烯酸甲酯(methyl acrylate)、N-乙烯基吡咯烷酮(N-Vinylpyrrolidone)以重量比76:(9.5):(9.5):5的比例搅拌混合。所得的丙烯腈共聚物,命名为P(AN-VAc-MA-NVP)。
实施例8-5:P(AN-VAc-MA-DMAA)的制备
反应流程同上但将反应单体改为丙烯腈(acrylonitrile)、乙酸乙烯酯(Vinylacetate)、丙烯酸甲酯(methyl acrylate)、N,N-二甲基丙烯酰胺以重量比80:(7.5):(7.5):5的比例搅拌混合。所得的丙烯腈共聚物,命名为P(AN-VAc-MA-DMAA)。
上述实施例8-1~8-5的共聚高分子的平均分子量介于10,000~1,500,000之间。于一实施方式中,实施例8-1~8-5的共聚高分子可借由溶液聚合、活性聚合、乳化聚合与分散聚合等方法形成共聚物。
实施例9
实施例9-1:制备各别以实施例8-1~8-5的共聚高分子作为粘着剂的锂镍钴锰氧(Li(NiCoMn)O2)正极极片
分别将实施例8-1~8-5所制备的共聚高分子作为粘着剂,与商用碳粉(Super P),商用锂镍钴锰氧(Li(NiCoMn)O2)(BASF)以重量比2.5:2.5:95的比例混合并以NMP作为溶剂,以旋转搅拌机(海裕)搅拌1小时。将搅拌完成的浆料以自动涂布机(elcometer,3570)涂布在铝箔上后,置入真空烘箱升温至100℃,加热24小时后取出,以碾压机滚压极片,即可得分别含有实施例8-1~8-5的共聚高分子的磷酸锂铁正极。
实施例9-2:含共聚高分子正极的锂离子电池的充放电测试
将实施例9-1所制备的正极极片,分别以钮扣型电池形式组装。首先,将商用聚丙烯(Polypropylene,PP)膜作为隔离层置于上述锂镍钴锰氧(Li(NiCoMn)O2)正极与锂金属负极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含共聚高分子的正极锂离子半电池的充放电效能。电位设定范围为2.8~4.2V,充电电流值设定为0.1C,放电电流值设定为0.1C、1C、3C、5C,结果如下表所示。
表19:含实施例8-1的共聚高分子的正极半电池在不同充放电流值下电容量
表20:含实施例8-2的共聚高分子的正极半电池在不同充放电流值下电容量
表21:含实施例8-3的共聚高分子的正极半电池在不同充放电流值下电容量
表22:含实施例8-4的共聚高分子的正极半电池在不同充放电流值下电容量
表23:含实施例8-5的共聚高分子的正极半电池在不同充放电流值下电容量
比较例3-1:P(AN-MA-Am-MAALi)的制备
将反应单体丙烯腈(acrylonitrile)、丙烯酸甲酯(methyl acrylate)、丙烯酰胺(Acrylamide)、丙烯酸甲酯锂(Lithiated methyl acrylate)以重量比84:6:6:4的比例搅拌混合,再加入过硫酸铵(Ammonium persulfate,APS)起始剂于水中。加热至60℃。反应12小时后,析出的产物以离心过滤法过滤,取下白色固体真空烘箱烘干24小时,所得的丙烯腈共聚物,命名为P(AN-MA-Am-MAALi)。
比较例3-2:P(AN-MA-Am)的制备
依上述制程将反应单体改变为丙烯腈(acrylonitrile)、丙烯酸甲酯(methylacrylate)、丙烯酰胺(Acrylamide)重量比84:4:12的比例搅拌混合。所得的丙烯腈共聚物,命名为P(AN-MA-Am)。
比较例3-3:P(AN-MA-Am)II的制备
依上述制程将反应单体改变为丙烯腈(acrylonitrile)、丙烯酸甲酯(methylacrylate)、丙烯酰胺(Acrylamide)重量比91:4:5的比例搅拌混合。所得的丙烯腈共聚物,命名为P(AN-MA-Am)II。
上述比较例3-1~3-3的共聚高分子的平均分子量介于10,000~1,500,000之间。于一实施方式中,比较例3-1~3-3的共聚高分子可借由溶液聚合、活性聚合、乳化聚合与分散聚合等方法形成共聚物。
比较例3-4:P(AN-MA-Am-MAALi)II的制备
依上述制程将反应单体改变为丙烯腈(acrylonitrile)、丙烯酸甲酯(methylacrylate)、丙烯酰胺(Acrylamide)、丙烯酸甲酯锂(Lithiated methyl acrylate)重量比84:4:8:4的比例搅拌混合。但此比较例无法成功制备。
比较例4
比较例4-1:制备各别以比较例3-1~3-4的共聚高分子作为粘着剂的锂镍钴锰氧(Li(NiCoMn)O2)正极极片
分别将比较例3-1~3-4所制备的共聚高分子作为粘着剂,与商用碳粉(Super P),商用锂镍钴锰氧(Li(NiCoMn)O2)(BASF)以重量比2.5:2.5:95的比例混合并以NMP作为溶剂,以旋转搅拌机(海裕)搅拌1小时。将搅拌完成的浆料以自动涂布机(elcometer,3570)涂布在铝箔上后,置入真空烘箱升温至100℃,加热24小时后取出,以碾压机滚压极片,即可得分别含有比较例3-1~3-4的共聚高分子的磷酸锂铁正极。
比较例4-2:含共聚高分子正极的锂离子电池的充放电测试
将比较例4-1所制备的正极极片,分别以钮扣型电池形式组装。首先,将商用聚丙烯(Polypropylene,PP)膜作为隔离层置于上述锂镍钴锰氧(Li(NiCoMn)O2)正极与锂金属负极之间。以小电流自动化充放电测试系统(AcuTech Systems,BAT-750B)量测含共聚高分子的正极锂离子半电池的充放电效能。电位设定范围为2.8~4.2V,充电电流值设定为0.1C,放电电流值设定为0.1C、1C、3C、5C,结果如下表所示。
表24:含比较例3-1的共聚高分子的正极半电池在不同充放电流值下电容量
表25:含比较例3-2的共聚高分子的正极半电池在不同充放电流值下电容量
表26:含比较例3-3的共聚高分子的正极半电池在不同充放电流值下电容量
表27:含比较例3-4的共聚高分子的正极半电池在不同充放电流值下电容量
测试例1:实施例8-1~8-5与比较例3-1~3-4的共聚高分子的示差扫描热析法(differential scanning calorimetry,DSC)比较
取实施例8-1~8-5与比较例3-1~3-4的共聚高分子干燥后样品2~5mg,且DCS测定范围为-20~150℃,并以每分钟10℃为升温条件,观测其玻璃转移温度,其结果如图4~图11所示。
如图4~图11所示,由实施例8-1~8-5与比较例3-1~3-3比较可得,本发明的实施例8-1~8-5相较于比较例3-1~3-3具有较低的玻璃转移温度,本发明实施例8-1~8-5的玻璃转移温度皆在40~80℃之间,但相较之下,比较例3-1~3-3的玻璃转移温度皆在100~120℃之间,代表本发明的实施例8-1~8-5具有较佳的可挠性与加工性,因此在制作极片时可具较佳的辗压密度与卷绕性。
综合上述实施例及比较例的测试结果可理解,本发明的能量储存装置于阳极、阴极及隔离层中的至少一个包含共聚高分子,且该共聚高分子是丙烯腈与乙酸乙烯酯经聚合反应后所形成的共聚物或其衍生物。借此,可使应用该共聚高分子的能量储存装置具有较佳的充放电性质,可有效地延长能量储存装置的效率及寿命。
实施例8-1~8-5的共聚高分子借由包含衍生自乙酸乙烯酯的单体,可使其具有较低的玻璃转移温度,且具有较佳的可挠性与加工性。相较之下,比较例3-1~3-3的共聚高分子由于未包含衍生自乙酸乙烯酯的单体,使其具有较高的玻璃转移温度,且可挠性与加工性不佳。
本发明在上文中已以较佳实施例揭露,然熟悉本项技术者应理解的是,该实施例仅用于描绘本发明,而不应解读为限制本发明的范围。应注意的是,凡是与该实施例等效的变化与置换,均应设为涵盖于本发明的范畴内。因此,本发明的保护范围当以权利要求书所界定的为准。
Claims (8)
2.根据权利要求1所述的能量储存装置,其特征在于,
GIII衍生自含有反应性官能基的单体,其中该含有反应性官能基的单体选自由丙烯酸甲酯、甲基丙烯酸缩水甘油酯、丙烯酸缩水甘油酯、乙烯基环氧环己烷、甲基丙烯酸2-(2-环氧乙烷基甲氧基)乙酯、甲基丙烯酸羟乙酯、烯丙基胺及乙烯胺所组成的组;
GIV衍生自含有乙烯基的单体,其中该含有乙烯基的单体选自由丙烯酰胺、N-乙烯基吡咯烷酮、N,N-二甲基丙烯酰胺、丙烯酸异辛酯、N-乙烯基吡咯烷酮、氯乙烯、二氯乙烯、溴乙烯、丙烯酸丁酯、丙烯酸异丁酯、亚甲基丁二酸二丁酯、马来酸二甲酯、马来酸二乙酯、马来酸二丁酯、苯乙烯、丙烯酸甲酯、乙烯基吡啶、甲基丙烯酸甲酯、丁二烯及异戊二烯所组成的组。
3.根据权利要求1或2所述的能量储存装置,其特征在于,该能量储存装置是电池,且该两个电极包含:阳极及阴极。
4.根据权利要求3所述的能量储存装置,其特征在于,该能量储存装置的阳极含有活性物质、导电碳以及该共聚高分子,且该共聚高分子的含量占该阳极的0.01%~30%重量百分比,其中共聚高分子单独使用或与任一高分子混掺作为阳极粘着剂。
5.根据权利要求3所述的能量储存装置,其特征在于,该共聚高分子的含量占该阴极的0.01%~30%重量百分比,其中共聚高分子单独使用或与任一高分子混掺作为阴极粘着剂。
6.根据权利要求1或2所述的能量储存装置,其特征在于,该共聚高分子进一步与含氨基、异氰酸酯、羟基、羧酸基、咪唑基的化合物反应,或与牛磺酸、磺内酯或其衍生物中的一种或其组合进行反应,以获得改质或交联。
7.根据权利要求1或2所述的能量储存装置,其特征在于,该隔离层经由涂布浆料或配方所形成,其中,该共聚高分子的含量占该浆料或配方成分的0.1%~30%重量百分比。
8.根据权利要求1或2所述的能量储存装置,其特征在于,该共聚高分子与任一高分子混掺作为该能量储存装置的固态电解质,且该共聚高分子的含量占该固态电解质成分的0.1%~90%重量百分比。
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TWI740390B (zh) | 2021-09-21 |
US20200343594A1 (en) | 2020-10-29 |
CN111933864B (zh) | 2022-12-20 |
CN111933864A (zh) | 2020-11-13 |
US11271254B2 (en) | 2022-03-08 |
US11316206B2 (en) | 2022-04-26 |
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