CN1303135A - 用于锂电池的聚合物电解质薄膜 - Google Patents
用于锂电池的聚合物电解质薄膜 Download PDFInfo
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- 229910052744 lithium Inorganic materials 0.000 title claims description 8
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 title claims description 6
- 239000005518 polymer electrolyte Substances 0.000 title description 2
- 239000012528 membrane Substances 0.000 claims abstract description 11
- 229910010293 ceramic material Inorganic materials 0.000 claims abstract description 9
- 239000000203 mixture Substances 0.000 claims description 11
- 229920002239 polyacrylonitrile Polymers 0.000 claims description 11
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 9
- 239000002033 PVDF binder Substances 0.000 claims description 7
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 7
- 229920003229 poly(methyl methacrylate) Polymers 0.000 claims description 5
- 239000004926 polymethyl methacrylate Substances 0.000 claims description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 4
- 239000002159 nanocrystal Substances 0.000 claims description 4
- 239000011159 matrix material Substances 0.000 claims description 3
- 239000002202 Polyethylene glycol Substances 0.000 claims description 2
- 229920001328 Polyvinylidene chloride Polymers 0.000 claims description 2
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 2
- 229920001223 polyethylene glycol Polymers 0.000 claims description 2
- 229920000642 polymer Polymers 0.000 claims description 2
- 229920000307 polymer substrate Polymers 0.000 claims description 2
- 239000005033 polyvinylidene chloride Substances 0.000 claims description 2
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 2
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 2
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 2
- 239000000377 silicon dioxide Substances 0.000 claims description 2
- 150000003457 sulfones Chemical class 0.000 claims description 2
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 2
- 229920002554 vinyl polymer Polymers 0.000 claims description 2
- CQDGTJPVBWZJAZ-UHFFFAOYSA-N monoethyl carbonate Chemical compound CCOC(O)=O CQDGTJPVBWZJAZ-UHFFFAOYSA-N 0.000 description 7
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 6
- 229910013870 LiPF 6 Inorganic materials 0.000 description 5
- 239000002904 solvent Substances 0.000 description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 4
- 239000003792 electrolyte Substances 0.000 description 4
- 229910001416 lithium ion Inorganic materials 0.000 description 4
- 229910003002 lithium salt Inorganic materials 0.000 description 4
- 159000000002 lithium salts Chemical class 0.000 description 4
- XEKOWRVHYACXOJ-UHFFFAOYSA-N Ethyl acetate Chemical compound CCOC(C)=O XEKOWRVHYACXOJ-UHFFFAOYSA-N 0.000 description 3
- 229910013684 LiClO 4 Inorganic materials 0.000 description 3
- -1 LiPF 6 Chemical class 0.000 description 3
- 239000000919 ceramic Substances 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
- 239000000243 solution Substances 0.000 description 3
- 229910015015 LiAsF 6 Inorganic materials 0.000 description 2
- 229910013063 LiBF 4 Inorganic materials 0.000 description 2
- WYURNTSHIVDZCO-UHFFFAOYSA-N Tetrahydrofuran Chemical compound C1CCOC1 WYURNTSHIVDZCO-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- BGTOWKSIORTVQH-UHFFFAOYSA-N cyclopentanone Chemical compound O=C1CCCC1 BGTOWKSIORTVQH-UHFFFAOYSA-N 0.000 description 2
- 230000005518 electrochemistry Effects 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000012266 salt solution Substances 0.000 description 2
- 125000006091 1,3-dioxolane group Chemical class 0.000 description 1
- JWUJQDFVADABEY-UHFFFAOYSA-N 2-methyltetrahydrofuran Chemical compound CC1CCCO1 JWUJQDFVADABEY-UHFFFAOYSA-N 0.000 description 1
- YEJRWHAVMIAJKC-UHFFFAOYSA-N 4-Butyrolactone Chemical compound O=C1CCCO1 YEJRWHAVMIAJKC-UHFFFAOYSA-N 0.000 description 1
- 229910010093 LiAlO Inorganic materials 0.000 description 1
- 229910015645 LiMn Inorganic materials 0.000 description 1
- AYDQIZKZTQHYIY-UHFFFAOYSA-N OC(=O)C1(C)CC(C(O)=O)=CC=C1 Chemical compound OC(=O)C1(C)CC(C(O)=O)=CC=C1 AYDQIZKZTQHYIY-UHFFFAOYSA-N 0.000 description 1
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 1
- 229910021536 Zeolite Inorganic materials 0.000 description 1
- KXKVLQRXCPHEJC-UHFFFAOYSA-N acetic acid trimethyl ester Natural products COC(C)=O KXKVLQRXCPHEJC-UHFFFAOYSA-N 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 230000004888 barrier function Effects 0.000 description 1
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- IHLVCKWPAMTVTG-UHFFFAOYSA-N lithium;carbanide Chemical compound [Li+].[CH3-] IHLVCKWPAMTVTG-UHFFFAOYSA-N 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- 239000003791 organic solvent mixture Substances 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 229920006254 polymer film Polymers 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 239000010457 zeolite Substances 0.000 description 1
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- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
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Abstract
本发明涉及到包含陶瓷材料的凝胶状薄膜,并且是为了电化学池而设计的。
Description
本发明涉及包括陶瓷材料的凝胶状薄膜，并且是为电化学池而设计的。
锂离子电池对于移动用途是最好的保证体系之一。其使用的场合，范围从高级电子设备(例如移动电话，摄像和录像机)到电动汽车的电池。
这种电池由阴极，阳极，隔膜和非水电解质组成。典型的阴极包括Li(MnMez)2O4,Li(CoMez)O2,Li(CoNixMez)O2，或其它的锂夹杂和嵌入化合物。阳极可为锂金属、碳、石墨、石墨碳或其它的锂夹杂和嵌入化合物或合金。作为电解质，使用对质子惰性的溶剂中的锂盐溶液，该锂盐如LiPF6,LiBF4,LiClO4,LiAsF6,LiCF3SO3,LiN(CF3SO2)2或LiC(CF3SO2)3及其混合物。
众所周知，凝胶状薄膜通过在聚合物基质(例如聚丙烯腈)上固定液体锂盐溶液(例如，溶解在有机溶剂混合物中的锂盐)得到。JP10284091描述了由聚丙烯腈(PAN)和聚偏二氟乙烯(PVDF)制得的锂离子电池用聚合物薄膜。用LiMn2O4阴极，石墨阳极和聚丙烯腈基电解质的电池原型已为Abrsham等人所描述(电化学实践，Electrochemi.Acta,1998,2399-2412)。这种电池在室温下具有良好的电导率。
所述的薄膜在室温下电导率为10-3S cm-1。然而，它们在高于室温时的化学和机械的稳定性差。
Scrosati等人描述了沸石用于凝胶状薄膜(固态离子材料，SolidState Ionic Mater.,1994,111-117)。对锂金属表面上的薄膜的影响进行了研究。
Appetecchi等人(电化学科学杂志，J.Electrochemi.Soc.,1998,4126-4132)将陶瓷粉末如γ-LiAlO2添加到聚环氧乙烷基质中以便减少锂钝化作用的增加。然而，这种混合物有二个严重的缺点。最佳的操作温度，在80℃这太高了，其电导率为0.6-1.0×10-4S cm-1，太低了。
因此本发明的目的是提供一种具有改进的稳定性和锂离子电导率的电解质。
本发明的目的是通过使用聚合物基凝胶状薄膜实现的，该聚合物选自聚丙烯腈，聚甲基丙烯酸甲酯，聚偏二氯乙烯，聚乙烯基砜，聚二丙烯酸乙二醇酯，聚乙烯吡咯烷酮，聚偏二氟乙烯或其混合物，包含的陶瓷材料选自氧化铝，氧化硅，氧化钛和氧化锆以及其混合物。
发现纳米晶体的陶瓷粉末的加入导致体系的稳定性增加。该纳米晶体陶瓷材料添加的比例从薄膜重量的1％到9％，优选在5到7％之间。
所有电化学池用的常用导电盐和溶剂都可以用作电解质。所用的电解质可以是LiPF6,LiBF4,LiClO4,LiAsF6,LiCF3SO3,LiN(CF3SO2)2或LiC(CF3SO2)3及其混合物在对质子惰性的溶剂中的溶液，这些溶剂如EC,DMC,PC,DEC,BC,VC，环戊酮，环丁砜，DMS,3-甲基-1,3-噁唑烷-2-酮，γ-丁内酯，EMC,MPC,BMC,EPC,BEC,DPC,1,2-二乙氧基甲烷，THF，2-甲基四氢呋喃，1,3-二氧戊环，乙酸甲酯，乙酸乙酯及其混合物。
本发明的实施例说明如下。
根据导电盐的组成，一般有二种薄膜是合用的。使用LiPF6或LiClO4在碳酸乙酯/碳酸二甲酯(EC/DMC)混合物中的溶液，或LiC(CF3SO2)3(甲基锂)在EC/DMC中的溶液。
特别适用的凝胶状薄膜是以聚丙烯腈(PAN)，聚甲基丙烯酸甲酯(PMMA)或聚偏二氟乙烯(PVDF)为基的薄膜。使用纳米晶体陶瓷材料。特别优选使用Al2O3。
研究了以LiPF6作为导电盐和碳酸乙酯(EC)和碳酸二甲酯(DMC)作为溶剂的聚丙烯腈(PAN)薄膜的电导率。在高于室温的温度下，优选地在40℃和80℃之间，时间超过1600小时，测定了这种薄膜的电导率，与含有PAN,LiPF6,EC/DMC和Al2O3的薄膜进行比较。在没有陶瓷填充材料的情况下，发现在800小时以后电导率急剧下降。在Al2O3填充的薄膜情况下，观察到电导率保持不变。
这些凝胶状薄膜可以用于电化学池，优选用于电池，特别优选用于锂离子电池。
Claims (8)
1．一种聚合物基凝胶状薄膜，该聚合物选自聚丙烯腈，聚甲基丙烯酸甲酯，聚偏二氯乙烯，聚乙烯基砜，聚二丙烯酸乙二醇酯，聚乙烯吡咯烷酮，聚偏二氟乙烯或其混合物所组成的组，该薄膜包括选自氧化铝，氧化硅，氧化钛和氧化锆以及其混合物的陶瓷材料。
2．根据权利要求1的薄膜，其特征在于，它包含纳米晶体。
3．根据权利要求1或2的薄膜，其特征在于，它包含的陶瓷材料的浓度在薄膜重量的1和9％之间。
4．根据权利要求1至3中任一项的薄膜，其特征在于，该陶瓷材料的浓度在薄膜重量的5和7％之间。
5．根据权利要求1至4中任一项的薄膜，其特征在于，将聚丙烯腈，聚甲基丙烯酸甲酯，聚偏二氟乙烯或它们的混合物用作聚合物基质，并将氧化铝用作陶瓷材料。
6．根据权利要求1到5中任一项的凝胶状薄膜的用途，用于在温度为40℃到80℃之间时稳定电导率。
7．根据权利要求1到5中任一项的凝胶状薄膜的用途，用于电化学池。
8．根据权利要求7的凝胶状薄膜的用途，用于电池，包括锂二次电池。
Applications Claiming Priority (4)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| EP99121289 | 1999-10-26 | ||
| EP99121289.5 | 1999-10-26 | ||
| DE19951872.6 | 1999-10-28 | ||
| DE19951872A DE19951872A1 (de) | 1999-10-28 | 1999-10-28 | Polymer Elektrolyt-Membran zum Einsatz in Lithium Batterien |
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| Publication Number | Publication Date |
|---|---|
| CN1303135A true CN1303135A (zh) | 2001-07-11 |
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| Application Number | Title | Priority Date | Filing Date |
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| CN00131956A Pending CN1303135A (zh) | 1999-10-26 | 2000-10-26 | 用于锂电池的聚合物电解质薄膜 |
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| Country | Link |
|---|---|
| EP (1) | EP1096591A1 (zh) |
| JP (1) | JP2001155770A (zh) |
| KR (1) | KR20010060192A (zh) |
| CN (1) | CN1303135A (zh) |
| BR (1) | BR0005037A (zh) |
| CA (1) | CA2324127A1 (zh) |
| RU (1) | RU2000126671A (zh) |
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1302575C (zh) * | 2001-11-24 | 2007-02-28 | 三星Sdi株式会社 | 制备包含多相隔膜的锂二次电池的方法 |
| CN1327546C (zh) * | 2004-02-24 | 2007-07-18 | 株式会社巴川制纸所 | 电子部件用隔膜及其制造方法 |
| CN100341168C (zh) * | 2005-01-27 | 2007-10-03 | 河南环宇集团有限公司 | 聚合物锂离子电池的聚合物隔膜及其制备方法 |
| CN100343329C (zh) * | 2005-03-18 | 2007-10-17 | 西北工业大学 | 凝胶型聚甲基丙烯酸甲酯/有机累托石电解质及其制备方法 |
| CN101814631A (zh) * | 2009-02-23 | 2010-08-25 | 索尼公司 | 非水电解液组合物,非水电解液二次电池,和制造非水电解液二次电池的方法 |
| CN101150182B (zh) * | 2006-09-18 | 2011-12-07 | 深圳市比克电池有限公司 | 锂离子电池极片、电芯及电芯制备方法 |
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| DE10219423A1 (de) | 2002-05-02 | 2003-11-20 | Varta Microbattery Gmbh | Verfahren zur Herstellung eines galvanischen Elements |
| KR100659820B1 (ko) * | 2004-11-17 | 2006-12-19 | 삼성에스디아이 주식회사 | 리튬 이온 이차 전지 |
| KR100709860B1 (ko) | 2005-07-22 | 2007-04-23 | 삼성에스디아이 주식회사 | Ｓｉ함유 물질층 및 다공성막을 포함하는 전극 및 이를채용한 리튬 전지 |
| KR100886916B1 (ko) * | 2007-05-14 | 2009-03-09 | 부산대학교 산학협력단 | 높은 굴절률을 갖는 투명 고분자 나노 하이브리드 필름 및이의 제조방법 |
| KR102034720B1 (ko) * | 2011-06-23 | 2019-10-22 | 삼성전자주식회사 | 세라믹 입자, 이를 포함하는 고분자막 및 리튬전지, 및 상기 세라믹 입자의 제조방법 |
| US9525197B2 (en) | 2011-10-10 | 2016-12-20 | Toyota Motor Europe Nv/Sa | Stable non-aqueous electrolyte promoting ideal reaction process in rechargeable lithium-air batteries |
| CN102875919A (zh) * | 2012-09-27 | 2013-01-16 | 无锡宏昌五金制造有限公司 | 一种轻便洛阳铲 |
| CN107408655A (zh) | 2014-12-29 | 2017-11-28 | 赛尔格有限责任公司 | 用于锂离子二次电池的聚内酰胺涂覆的隔板膜及相关涂覆配方 |
| CN105047845A (zh) * | 2015-06-19 | 2015-11-11 | 深圳市星源材质科技股份有限公司 | 一种高介电常数的纳米复合涂层隔膜及其制备方法 |
| IT201800010452A1 (it) | 2018-11-20 | 2020-05-20 | Univ Degli Studi G Dannunzio | Materiali nanocompositi elettrofilati a base cu2o/carbone come anodi per batterie a litio |
| KR102524662B1 (ko) * | 2019-05-09 | 2023-04-20 | 주식회사 엘지에너지솔루션 | 바인더 수지 조성물 및 이를 포함하는 전기화학소자용 분리막 |
| WO2021148836A1 (en) | 2020-01-20 | 2021-07-29 | Toyota Motor Europe | Naphthalene based lithium compounds, a process for their preparation, their use as solid organic catalyst, and their use in rechargeable non-aqueous lithium-air battery cells |
| JP7438375B2 (ja) | 2020-01-20 | 2024-02-26 | トヨタ・モーター・ヨーロッパ | 固体有機触媒を備える充電可能な非水性リチウム空気電池セル |
| EP4290637A1 (en) | 2022-06-07 | 2023-12-13 | Toyota Jidosha Kabushiki Kaisha | Metal m-air battery cell comprising an organic multi redox mediator compound as soluble organic catalyst |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5893734A (ja) * | 1981-11-30 | 1983-06-03 | Asahi Chem Ind Co Ltd | 親水性ポリフツ化ビニリデン樹脂多孔膜の製造方法 |
| JPS60153903A (ja) * | 1984-01-23 | 1985-08-13 | Nok Corp | 限外口過膜の製造法 |
| AU9441498A (en) * | 1997-09-22 | 1999-04-12 | W.L. Gore & Associates Gmbh | An electrochemical energy storage means |
| AU2636999A (en) * | 1998-02-24 | 1999-09-15 | Ramot University Authority For Applied Research And Industrial Development Ltd. | Ion conductive matrixes and their use |
| JP3040757B1 (ja) * | 1998-11-09 | 2000-05-15 | 株式会社ジャパンエナジー | リチウム２次電池用セパレータ材料 |
-
2000
- 2000-10-14 EP EP00122498A patent/EP1096591A1/en not_active Withdrawn
- 2000-10-23 KR KR1020000062218A patent/KR20010060192A/ko not_active Application Discontinuation
- 2000-10-24 CA CA002324127A patent/CA2324127A1/en not_active Abandoned
- 2000-10-25 BR BR0005037-7A patent/BR0005037A/pt not_active Application Discontinuation
- 2000-10-25 RU RU2000126671/09A patent/RU2000126671A/ru not_active Application Discontinuation
- 2000-10-26 CN CN00131956A patent/CN1303135A/zh active Pending
- 2000-10-26 JP JP2000326338A patent/JP2001155770A/ja active Pending
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1302575C (zh) * | 2001-11-24 | 2007-02-28 | 三星Sdi株式会社 | 制备包含多相隔膜的锂二次电池的方法 |
| CN1327546C (zh) * | 2004-02-24 | 2007-07-18 | 株式会社巴川制纸所 | 电子部件用隔膜及其制造方法 |
| CN100341168C (zh) * | 2005-01-27 | 2007-10-03 | 河南环宇集团有限公司 | 聚合物锂离子电池的聚合物隔膜及其制备方法 |
| CN100343329C (zh) * | 2005-03-18 | 2007-10-17 | 西北工业大学 | 凝胶型聚甲基丙烯酸甲酯/有机累托石电解质及其制备方法 |
| CN101150182B (zh) * | 2006-09-18 | 2011-12-07 | 深圳市比克电池有限公司 | 锂离子电池极片、电芯及电芯制备方法 |
| CN101814631A (zh) * | 2009-02-23 | 2010-08-25 | 索尼公司 | 非水电解液组合物,非水电解液二次电池,和制造非水电解液二次电池的方法 |
| CN112635817A (zh) * | 2019-10-09 | 2021-04-09 | 成功大学 | 胶态电解质及其制作方法，以及锂电池 |
| CN112635817B (zh) * | 2019-10-09 | 2021-11-02 | 成功大学 | 胶态电解质及其制作方法，以及锂电池 |
Also Published As
| Publication number | Publication date |
|---|---|
| BR0005037A (pt) | 2001-06-19 |
| EP1096591A1 (en) | 2001-05-02 |
| KR20010060192A (ko) | 2001-07-06 |
| JP2001155770A (ja) | 2001-06-08 |
| CA2324127A1 (en) | 2001-04-26 |
| RU2000126671A (ru) | 2002-09-10 |
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