CN1800191B - 环状碳酸酯改性的有机硅化合物、无水电解溶液、二次电池和电容器 - Google Patents
环状碳酸酯改性的有机硅化合物、无水电解溶液、二次电池和电容器 Download PDFInfo
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- CN1800191B CN1800191B CN2005101373679A CN200510137367A CN1800191B CN 1800191 B CN1800191 B CN 1800191B CN 2005101373679 A CN2005101373679 A CN 2005101373679A CN 200510137367 A CN200510137367 A CN 200510137367A CN 1800191 B CN1800191 B CN 1800191B
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- Prior art keywords
- nonaqueous electrolyte
- electrolyte solution
- integer
- alkyl
- cyclic carbonate
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- 125000000217 alkyl group Chemical group 0.000 claims description 18
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- 239000011572 manganese Substances 0.000 description 1
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- KKQAVHGECIBFRQ-UHFFFAOYSA-N methyl propyl carbonate Chemical compound CCCOC(=O)OC KKQAVHGECIBFRQ-UHFFFAOYSA-N 0.000 description 1
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- 239000002912 waste gas Substances 0.000 description 1
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- 229910052726 zirconium Inorganic materials 0.000 description 1
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Abstract
一种环状碳酸酯改性的硅烷或硅氧烷与非水溶剂和电解质盐结合形成一种非水电解溶液,该非水电解溶液用于构成具有改进的温度和高输出特性的二次电池。
Description
技术领域
本发明涉及一种具有环状碳酸酯基团的新型有机硅化合物和包含此有机硅化合物的非水电解溶液。非水电解溶液适用于各种能量装置,典型地为二次电池和电化学电容器,典型地是双电层电容器,和特别是锂离子二次电池,该锂离子二次电池通过阳极和阴极间锂离子的迁移能够进行充电/放电。使用本发明非水电解溶液的电池具有改进的温度特性和高输出特性。
背景技术
由于其高能量密度,近年来锂离子二次电池日益地被用作膝上型计算机、移动电话、数码像机和数码摄影机的便携式可充电电源。人们还进行了大量的工作致力于锂离子二次电池或双电层电容器的开发,该锂离子二次电池用作电动汽车和混合动力汽车的辅助电源,这些汽车被期望达到作为对环境有益的汽车的实际可接受的水平,该对环境有益的汽车能够释放少量或不释放废气到空气中。
虽然其具有高性能,但是锂离子二次电池在严峻条件下、特别是在低温环境的放电性能和在短时间内需要大量电流的高输出水平下的放电性能不能令人满意。另一方面,双电层电容器也存在一些问题,包括不足的耐压和随时间电容的降低。大多数这类设备使用包括例如碳酸二甲酯和碳酸二乙酯作为主要成分的低闪点溶剂的非水电解溶液作为主要成分。如果在电池中出现热击穿,那么电解溶液可被蒸发和分解,引起电池的损坏或燃烧的风险。这就需要在电池中插入一个IC电路作为异常时中断电流的装置,并插入一个安全阀用于避免由于产生烃气体而导致电池中内压升高的危险。对电解溶液进行进一步的研究以改进其安全性、减轻重量和降低成本。
在这种情况下,针对具有高化学稳定和与电解溶液高相容性的聚醚改性的硅氧烷进行了研究。聚醚改性的硅氧烷能够彻底地溶解如LiPF6的电解质,同时由于其自身的表面活化能力,有助于湿润电极或隔板。公知地,仅仅百分之几的聚醚改性的硅氧烷的加入可提高充电/放电循环的性能。然而,这些效果并不充分。聚醚改性的硅氧烷具有较低的热稳定性并且由于相对高的熔点,其在低温下使用也存在问题。这样对具有高安全性和与电解溶液高相容性的添加剂存在一种需求。
可以参考JP-A 11-214032和JP-A 2000-58123,它们都对应于USP6,124,062,JP-A 2001-110455,和JP-A 2003-142157。
发明内容
本发明的目的是提供新型环状碳酸酯改性的有机硅化合物以替代现有技术的聚醚改性的硅氧烷。另一个目的是提供能够构成电池、尤其是二次电池的非水电解溶液,该二次电池具有在低温和高输出下改进的放电特性和高等级的安全性,以及提供一种电池,尤其是锂离子二次电池或诸如使用该非水电解溶液的双电层电容器的电化学电容器。
发明人已发现具有环状碳酸酯基团的改性的硅烷和硅氧烷可作为替代现有技术的聚醚改性的硅氧烷的新的改性化合物。当在二次电池或双电层电容器中使用包含环状碳酸酯改性的硅烷或硅氧烷的非水电解溶液时,改进了电池或电容器的充电/放电特性和安全性。
具体地,本发明提供了一种选自具有下面通式(1)至(3)的环状碳酸酯改性的硅烷和硅氧烷的有机硅化合物:
R1 (4-a)R2 aSi (1)
其中R1可以是相同的或不同的,为选自任选卤素取代的1至30个碳原子的烷基,芳基,芳烷基,氨基取代的烷基,羧基取代的烷基和烷氧基的有机基团,a是1至4的整数,b是0至3的整数,c是0至3的整数,x和y各自为0或1,但须满足当c为0时1≤x+y,d是0至5的整数,e是1至6的整数,满足3≤d+e≤6。R2是具有化学式(4)的环状碳酸酯基:
本发明还提供了一种非水电解溶液,其包含作为必要组分的非水溶剂、电解质盐和一种或多种选自具有通式(1)至(3)的环状碳酸酯改性的硅烷和硅氧烷的有机硅化合物。
此外,本发明提供了一种包含非水电解溶液的二次电池,电化学电容器和锂离子二次电池。
包含非水电解溶液的电池表现出改进的温度特性和高输出特性,该非水电解溶液包含选自环状碳酸酯改性的硅烷和硅氧烷的有机硅化合物。
附图说明
图1是具有化学式(i)的化合物的NMR光谱。
图2是具有化学式(i)的化合物的IR吸收光谱。
图3是具有化学式(ii)的化合物的NMR光谱。
图4是具有化学式(ii)的化合物的IR吸收光谱。
具体实施方案
本发明的环状碳酸酯改性的有机硅化合物是具有下面通式(1)至(3)的硅烷和硅氧烷:
R1 (4-a)R2 aSi (1)
其中R1可以是相同的或不同的,为卤素可部分取代的1至30个碳原子的烷基,芳基,芳烷基,氨基取代的烷基,羧基取代的烷基,或烷氧基。实例包括烷基,如甲基、乙基、丙基、丁基、戊基、己基、庚基、辛基、壬基和癸基;环烷基,如环戊基和环己基;芳基,如苯基和甲苯基;芳烷基,如苄基和苯乙基;以及氨基取代的烷基,如3-氨基丙基和3-[(2-氨基乙基)氨基]丙基和羧基取代的烷基,如3-羧基丙基。卤素原子取代的烷基也是有益的,也就是其中一些氢原子被卤素原子取代的烷基,如三氟丙基和九氟辛基。示例性的烷氧基包括甲氧基、乙氧基、丙氧基和异丙氧基。这其中,优选1至6个碳原子的一价烃基。烷基和氟代烷基是更优选的。甲基或乙基是最优选的。优选至少80%的R1是甲基或乙基。
R2是具有化学式(4)的环状碳酸酯基。
下标“a”是1至4的整数,在a=3或4的情况下,相对地增加了碳酸酯基的含量,而损坏了硅烷或硅氧烷的自身特性。出于此原因,优选a为1或2,最优选a为1。
下标b和c是满足0≤b≤3和0≤c≤3的整数。因此0≤b+c≤6。如果表示聚合程度的下标b和c大于3,碳酸酯改性的硅氧烷具有增加的粘度,这可导致电解溶液中离子迁移率的降低。此外,碳酸酯改性的硅氧烷可变得与电解溶液的相容峨并抑制电解质的稳定溶解。因此优选b和c满足0≤b+c≤3,更优选0≤b+c≤2,x和y分别为0或1,但必须是当c=0时1≤x+y,表明x+y等于1或2。下标d和e是满足0≤d≤5、1≤e≤6和3≤d+e≤6的整数。如果表示聚合程度的下标d和e大于这个范围,碳酸酯改性的硅氧烷就具有增加的粘度,这可导致电解溶液中离子迁移率的降低。此外,碳酸酯改性的硅氧烷可变得与电解溶液的相容性较差并抑制电解质的稳定溶解。因此,优选d和e满足0≤d≤3和1≤e≤3,更优选0≤d≤3和1≤e≤2。
下面给出了具有通式(1)至(3)的环状碳酸酯改性的硅烷和环状碳酸酯改性的硅氧烷的示例性实例。
通过具有与硅结合氢原子(SiH基团)的有机氢硅烷或有机氢硅氧烷与具有碳碳双键的环状碳酸酯的加成反应,能够获得本发明的环状碳酸酯改性硅烷和硅氧烷。例如,通过作为承载有SiH基的硅氧烷的五甲基二硅氧烷与碳酸乙烯基亚乙酯(或4-乙烯基-1,3-二氧戊环-2-酮)(4-viny1-1,3-dioxolan-2-one)的加成反应,能够获得通式(ii)的化合物。
以在铂或铑催化剂存在下实现加成反应为宜。在此使用的适当的催化剂包括氯铂酸、乙醇改性氯铂酸和氯铂酸乙烯基硅氧烷复合物。可以加入助催化剂或PH调节剂如乙酸钠或柠檬酸钠。所使用的催化剂的量为催化的量,优选铂或铑基于含SiH基的硅氧烷和碳酸乙烯基亚乙酯的总重量计为至多50ppm,更优选至多20ppm。
如果需要,加成反应可以在有机溶剂中进行,适宜的有机溶剂包括脂肪醇,如甲醇、乙醇、2-丙醇和丁醇;芳烃如甲苯和二甲苯;脂肪或脂环烃如正戊烷、正己烷和环己烷;和卤化烃,如二氯甲烷、氯仿和四氯化碳。加成反应条件没有特别的限制。典型地在回流下进行加成反应约1至10小时。
另一方面,本发明提供了一种包含上述环状碳酸酯改性的有机硅化合物的非水电解溶液。在此,除了环状碳酸酯改性的有机硅化合物以外,非水电解溶液还包含非水溶剂和一种电解质盐。
在非水电解溶液中,环状碳酸酯改性的有机硅化合物优选存在的量为至少0.001体积%。少于0.001体积%的有机硅化合物不能实现所需要的效果。优选的量为至少0.1体积%。有机硅化合物含量的上限随着在非水电解溶液中所使用的溶剂的特定类型而变化,但是其应该被确定以使非水电解溶液内的锂离子的迁移为实际可接受的水平或之上。有机硅化合物的含量通常至多占非水电解溶液的80体积%,优选至多占50体积%,和更优选至多占50体积%。可替代地,可以从非水电解溶液中除去挥发性溶剂,也就是,有机硅化合物的量为非水电解溶液体积的100%。
对环状碳酸酯改性的有机硅化合物的粘度没有特别的限制。为达到非水电解溶液中锂离子的平稳迁移,有机硅化合物优选具有至多500mm2/s的粘度,更优选至多为100mm2/s,甚至更优选至多50mm2/s,其粘度在25℃下用Cannon-Fenske粘度计测得。尽管不是关键性的,但粘度的下限通常为至少0.1mm2/s。
本发明的非水电解溶液进一步包含电解质盐和非水溶剂。在此所使用的典型的电解质盐为轻金属盐,包括碱金属盐如锂、钠和钾,碱土金属盐如镁和钙,以及铝盐。对于特定的目的可选择一种或多种盐。锂盐的实例包括LiBF4、LiClO4、LiPF6、LiAsF6、CF3SO3Li、(CF3SO2)2NLi、C4F9SO3Li、CF3CO2Li、(CF3CO2)2NLi、C6F5SO3Li、C8F17SO3Li、(C2F5SO2)2NLi、(C4F9SO2)(CF3SO2)NLi、(FSO2C6F4)(CF3SO2)NLi、((CF3)2CHOSO2)2NLi、(CF3SO2)3CLi、(3,5-(CF3)2C6F3)4BLi、LiCF3、LiAlCl4和C4BO8Li。这些盐可以单独使用或以两种或两种以上的混合物的形式使用。
从电导率方面考虑,电解质盐优选以0.5至2.0摩尔/升非水电解溶液的浓度存在。电解溶液优选具有在25℃下至少0.01S/m的电导率,该电导率可以通过电解质盐的类型和浓度来调节。
在此所使用的非水溶剂没有特别的限制,只要它能用作非水电解溶液即可。适宜的溶剂包括质子惰性的高介电常数溶剂,如碳酸亚乙酯、碳酸亚丙酯、碳酸亚丁酯和γ-丁内酯;和质子惰性的低粘度溶剂如碳酸二甲酯、碳酸乙基甲酯、碳酸二乙酯、碳酸甲基丙基酯、碳酸二丙酯、二乙醚、四氢呋喃、1,2-二甲氧基乙烷、1,2-二乙氧基乙烷、1,3-二氧戊环、环丁砜、甲基环丁砜、乙腈、丙腈、苯甲醚,乙酸酯如乙酸甲酯,以及丙酸酯。使用适当比例混合的质子惰性的高介电常数溶剂和质子惰性的低粘度溶剂的混合物也是令人满意的。使用包含咪唑鎓、铵、吡啶鎓阳离子的离子性液体也是可以接受的。对于相反的阴离子没有特别的限制,并且包含BF4-,PF6和(CF3SO2)2N-。离子性液体可以与前述非水溶剂以混合物形式使用。
在需要固体电解质或凝胶电解质的地方,可以包括以聚合物形式的硅凝胶、硅聚醚凝胶、丙烯酸凝胶、丙烯腈凝胶、聚偏二氟乙烯等。这些成分可以在浇铸前或浇铸后聚合。它们可以单独使用或以混合物的形式使用。
如果需要,可以将各种添加剂加入到本发明的非水电解溶液中。实例包括用于改进循环周期的添加剂如碳酸亚乙烯酯、碳酸甲基亚乙烯基酯、碳酸乙基亚乙烯基酯和碳酸4-乙烯基亚乙基酯,用于抑制过量充电而加入的添加剂如联苯、烷基联苯、环己基苯、叔丁基苯、二苯基醚和苯并呋喃,和用于除酸和除水目的的各种碳酸酯化合物,酸酐、含氮和含硫化合物。
本发明进一步的实施方案是一种包含阳极、阴极、隔板和电解溶液的二次电池,其中使用上述非水电解溶液作为电解溶液。
阳极活性材料包括能够吸收和释放锂离子的氧化物和硫化物。它们可以单独使用或以混合物的形式使用。实例包括除了锂以外的金属氧化物和硫化物,如TiS2、MoS2、NbS2、ZrS2、VS2、V2O5、MoO3、Mg(V3O8)2,以及锂及含锂的复合氧化物。复合金属如NbSe2也是可以使用的。为增加能量密度,优选基于LipMeetO2的锂复合氧化物,其中Met优选为钴、镍、铁和锰中的至少一种元素,并且p值的范围是0.05≤p≤1.10。锂复合氧化物的示例性实例包括LiCoO2、LiNiO2、LiFeO2和具有层状结构的LiqNirCo1-rO2(其中q和r的值随着电池充电/放电状态而改变,并且通常是在这个范围内:0≤q<1和0.7<r≤1),具有尖晶石结构的LiMn2O4,以及菱形的LiMnO2。也可使用适用于高压操作的大体上为尖晶石类的锰化合物LiMetsMn1-sO4(0<s<1),其中Met是钛、铬、铁、钴、镍、铜、锌等。
应该注意到,例如,根据所需的组份通过研磨和混合锂的碳酸盐、硝酸盐、氧化物或氢氧化物与过渡金属的碳酸盐、硝酸盐、氧化物或氢氧化物,并在氧气中于600至1000℃的温度下烧结而制备上述的锂复合氧化物。
也可使用有机材料作为阳极活性材料。实例包括如聚乙炔、聚吡咯、聚对亚苯、聚苯胺、聚噻吩、聚并苯(polyacene)和聚硫。
可以吸收和释放锂离子的阴极材料包括含碳材料、金属元素和类金属元素、金属复合氧化物,以及聚合物如聚乙炔和聚吡咯。
适宜的含碳材料根据碳化方法分类,并包括碳素类和通过气相方法合成的合成石墨类,如乙炔黑、热解碳和天然石墨;通过液相方法合成的碳素类包括如石油焦炭和沥青炭焦的焦炭;通过烧窑聚合物、木材、酚醛树脂和碳膜获得的热解碳;和通过固相方法合成的碳素类如木炭、玻璃碳(vitreous carbons)和碳纤维。
在能够吸收和释放锂离子的阴极材料中还包括以元素、合金或化合物形式存在的金属元素和能够与锂形成合金的类金属元素。它们的状态包括固体溶液、共熔化合物和具有两种或多种任选共存状态的金属互化物。它们可以单独使用或两种或以两种以上混合物的形式使用。
适宜的金属元素和类金属元素的实例包括锡、铅、铝、铟、硅、锌、铜、钴、锑、铋、镉、镁、硼、镓、锗、砷、硒、碲、银、铪、锆和钇。特别地,优选以元素、合金或化合物形式的4B族的金属元素。更优选的是硅和锡或其合金或化合物。它们可以是结晶型的或无定形的。
这些合金和化合物的示例性实例包括LiAl、AlSb、CuMgSb、SiB4、SiB6、Mg2Si、Mg2Sn、Ni2Si、TiSi2、MoSi2、CoSi2、NiSi2、CaSi2、CrSi2、Cu5Si、FeSi2、MnSi2、NbSi2、TaSi2、VSi2、WSi2、ZnSi2、SiC,复合物Si/SiC,Si3N4、Si2N2O、SiOv(其中0<v≤2),复合物SiO/C、SnOw(其中0<w≤2)、SnSiO3、LiSiO和LiSnO。
在阳极和阴极的制备中可以使用任何需要的方法。通常,通过将活性材料、粘结剂、导电试剂等加入到溶剂中形成料浆,然后将料浆施加到电流收集板上,干燥并压制粘合,来制备电极。在此所使用的粘结剂通常选自聚偏二氟乙烯、聚四氟乙烯、苯乙烯丁二烯橡胶、异戊二烯橡胶和各种聚酰亚胺树脂。在此所使用的导电试剂通常选自含碳材料如石墨和碳黑,和金属材料如铜和镍。作为电流收集器,通常使用铝和铝合金作为阳极,使用金属如铜、不锈钢和镍以及它们的合金作为阴极。
对于设置在阳极和阴极间的隔板没有特别的限制,只要它相对电解溶液是稳定的并且保持溶液有效即可。通常,大多数隔板是多孔板或如聚乙烯和聚丙烯等的聚烯烃的无纺织物。也可使用多孔玻璃和陶瓷。
电池可以采用任何所需的形状。通常电池是硬币形的,其中将被冲压成硬币形的电极和隔板堆叠起来,或者电池是圆柱形的,其中电极板和隔极为螺旋地缠绕。
本发明的非水电解溶液也可用于包含电极、隔板和电解溶液的电化学电容器中,特别是双电层电容器或拟双电层电容器,不对称电容器和氧化还原电容器。
电容器中至少一个电极为主要由含碳材料构成的可极化的电极。可极化电极通常是由含碳材料、导电试剂和粘结剂形成。根据与用于锂二次电池相同的组成来制备可极化电极。例如,通过混合粉末或纤维状的活性碳与如碳黑或乙炔黑等的导电试剂,加入聚四氟乙烯作为粘结剂,并将混合物施加或压制到不锈钢或铝的电流收集器上,来制备可极化电极。类似地,隔板和电解溶液提供了高离子渗透材料,并且能够以大致相同的方式使用锂二次电池中所用的材料。其形状可以是硬币形、圆柱形或矩形的。
实施例
下面给出本发明的实施例用于进一步地解释本发明,但不能将其解释为要对本发明的限制。在25℃下使用Cannon-Fenske粘度计测量粘度(mm2/s)。
制备实施例1
具有化学式(i)的化合物的合成
将103g的碳酸乙烯亚乙酯、100g的甲苯和0.05g的含0.5%重量的氯铂酸的甲苯溶液加入到安装有搅拌器、温度计和回流冷凝器的反应器中。在80℃下搅拌并缓慢地将100g三乙基硅烷滴加到混合物中。当末端不饱和基团与SiH基团的摩尔比为约1.05时,发生发应。滴加完成后,在100℃下使反应溶液维持2小时以完成反应。将反应溶液在真空中精确分馏,在148℃/7Pa下收集馏液。以产率49%获得具有化学式(i)的碳酸酯改性的硅烷。其具有17mm2/s的粘度,1.006的比重,和用气相色谱法分析得出的99.1%的纯度。用重质氯仿作为测量溶剂通过1H-NMR进行测量,峰值出现于:0.47ppm(8H,m),0.88ppm(9H,t),1.67ppm(2H,m),4.04ppm(1H,dd),4.48ppm(1H,dd)和4.61ppm(1H,m),如图1所示。从图2中可见,用IR分析,在1807cm-1处可以观察到一个羰基的强信号。利用这些数据,可以确定产品为目标碳酸酯。
具有化学式(ii)化合物的合成
将100g的碳酸乙烯基亚乙酯、100g的甲苯和0.05g的含0.5%重量的氢氯铂酸的甲苯溶液加入到安装有搅拌器、温度计和回流冷凝器的反应器中。在100℃下搅拌并缓慢地将130g五甲基二硅氧烷滴加到混合物中。当最终不饱和基团与SiH基团的摩尔比为约1.0时,发生发应。滴加完成后,在80℃下使反应溶液维持2小时以完成反应。将反应溶液在真空中精确分馏,在123℃/12Pa下收集馏液。以产率52%获得具有化学式(ii)的碳酸酯改性的硅氧烷。其具有9.3mm2/s的粘度,0.996的比重,和用气相色谱法分析得出的99.5%的纯度。用重质丙酮作为测量溶剂通过1H-NMR进行测量,峰值出现于:0.10ppm(15H,s),0.55ppm(2H,m),1.78ppm(2H,m),4.15ppm(1H,dd),4.59ppm(1H,dd)和4.78ppm(1H,m),如图3所示。从图4中可见,用IR分析,在1807cm-1处可以观察到一个羰基强信号。利用这些数据,可以确定产品为目标碳酸酯。
通过根据在具有结构式(ii)化合物的合成中所使用的相同的组成进行反应,并使用具有与硅键合的氢原子(SiH基)的相应的有机氢化聚硅氧烷来合成具有化学式(iii)到(vii)的化合物。
【非水电解溶液的制备】
通过将具有化学式(i)至(vii)的硅氧烷溶解到以在表1中所示的比例的碳酸乙酯(EC)和碳酸二乙酯(DeC)的混合物中,并进一步在其中溶解1摩尔/升浓度的LiPF6,来制备非水电解溶液。作为对照,制备了不含硅氧烷的非水电解溶液,和加入了具有10体积%和20体积%的聚醚改性的硅氧烷作为替代的非水电解溶液。
注意到,聚醚改性的硅树脂公开在JP-A 11-214032中并具有下面的化学式:
【电池材料的制备】
所使用的阳极材料为使用LiCoO2作为活性材料和用铝箔作为电流收集器(商品名为Pioxcel C-100,Pionics有限公司提供)的单层板。所使用的阴极材料为用石墨作为活性材料和用铜箔作为电流收集器(商品名为PioxcelA-100,Pionics有限公司提供)的单层板。所使用的隔板为聚烯烃的多孔膜(商品名Celgard 2400,Celgard有限公司提供)。
【电池装配】
将2032硬币型电池装配在氩气覆盖的干燥盒子中,使用前述的电池材料,也可作为阳极导体的不锈钢外壳,也可作为阴极导体的不锈钢密封板,和绝缘的垫片。
【电池测试(低温特性)】
在25℃下重复充电步骤(最多4.2伏、并伴随着0.6mA的稳定电流)和放电步骤(最低2.5伏、并伴随着0.6mA的稳定电流)10次循环,然后同样地在5℃下重复充电/放电步骤。假如在25℃下第10次循环的放电容量是100,那么计数直到在5℃下放电容量降低至80的重复循环次数。
【电池测试(高输出特性)】
在25℃下重复充电步骤(最多4.2伏、并伴随着0.6mA的稳定电流)和放电步骤(最低2.5伏、并伴随着0.6mA的稳定电流)5次循环,然后在保持充电条件不变、但放电电流增加到5mA的情况下,同样地重复充电/放电步骤5次循环。这两种类型的充电/放电操作交替地重复进行。假如在初始6mA的充电/放电操作在第5次循环时放电容量为100,那么计数直到放电容量降低至80的重复循环次数。
结果在表2中示出。
表2
低温测试(循环数) | 高输出测试(循环数) | |
实施例1 | 228 | 206 |
实施例2 | 202 | 166 |
实施例3 | 215 | 180 |
实施例4 | 232 | 193 |
实施例5 | 185 | 171 |
实施例6 | 208 | 178 |
实施例7 | 218 | 197 |
实施例8 | 181 | 166 |
实施例9 | 188 | 175 |
对照例1 | 85 | 93 |
对照例2 | 14 | 9 |
对照例3 | 8 | 6 |
由表2的结果可见,与对照例1的不含碳酸酯改性的硅烷或硅氧烷及对照例2和3的使用聚醚改性的硅树脂相比,在本发明的范围内使用碳酸酯改性的硅烷或硅氧烷的电池表现出改进的低温和高输出特性。
Claims (18)
1.一种有机硅化合物,其选自具有下面通式(3)的环状碳酸酯改性的硅氧烷:
其中R1分别是选自任选卤素取代的1至30个碳原子的烷基、芳基、芳烷基、氨基取代的烷基、羧基取代的烷基和烷氧基的有机基,d是0至5的整数,e是1至6的整数,同时满足3≤d+e≤6,并且R2是具有化学式(4)的环状碳酸酯基:
3.权利要求2所述的非水电解溶液,其中通式(1)至(3)中的R1是1至6个碳原子的单价烃基。
4.权利要求2所述的非水电解溶液,其中有机硅化合物是以全部非水电解溶液的至少0.001体积%的量存在。
5.权利要求2所述的非水电解溶液,其中所述电解质盐是锂盐。
6.一种二次电池,其包含权利要求2的非水电解溶液。
7.一种电化学电容器,其包含权利要求2的非水电解溶液。
8.一种锂离子二次电池,其包含权利要求2的非水电解溶液。
9.权利要求2所述的非水电解溶液,其中所述有机硅化合物是至少一种选自以下式(i)至(vii)所示化合物的化合物:
13.权利要求12的非水电解溶液,其中通式(1)至(3)中的R1是1至6个碳原子的单价烃基。
14.权利要求12所述的非水电解溶液,其中有机硅化合物是以全部非水电解溶液的至少0.001体积%的量存在。
15.权利要求12所述的非水电解溶液,其中所述电解质盐是锂盐。
16.一种二次电池,其包含权利要求12的非水电解溶液。
17.一种电化学电容器,其包含权利要求12的非水电解溶液。
18.一种锂离子二次电池,其包含权利要求12的非水电解溶液。
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JP2005233232A JP4650625B2 (ja) | 2004-10-15 | 2005-08-11 | 環状カーボネート変性有機ケイ素化合物、それを含有する非水電解液並びに二次電池及びキャパシタ |
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