CN1329373A - 锂蓄电池 - Google Patents

锂蓄电池 Download PDF

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CN1329373A
CN1329373A CN01121105A CN01121105A CN1329373A CN 1329373 A CN1329373 A CN 1329373A CN 01121105 A CN01121105 A CN 01121105A CN 01121105 A CN01121105 A CN 01121105A CN 1329373 A CN1329373 A CN 1329373A
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lithium
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CN1222071C (zh
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崔允硕
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Samsung SDI Co Ltd
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Abstract

公开一种含锂阴极、阳极、隔板和电解质的锂电池。锂阴极的制备是通过在惰性气氛中熔融锂金属而制成液体锂并在集电器上涂覆液体锂。阳极包括阳极活性物质、导电性物质和粘合剂。隔板置于阳极和阴极之间;电解质浸没在阳极和阴极以及隔板中,并且所述电解质包括锂盐和有机溶剂。

Description

锂蓄电池
                          相关文献
本申请基于2000年6月13日在韩国工业产权局提出的2000-32515号申请，其内容在此引入作为参考文献。
                          发明背景
(a)发明领域
本发明涉及锂蓄电池，更准确地说，涉及具有均匀涂覆活性物质的电极的锂蓄电池。
(b)相关技术的描述
锂-硫蓄电池使用硫基化合物作为阳极活性物质，而锂金属、其合金或碳基化合物作为阴极活性物质。在阴极中，锂金属充电时沉积，放电时再氧化成为锂离子。碳基化合物是能使碱金属如锂或金属离子如锂离子掺入或脱出的化合物。锂-硫蓄电池使用一种溶解多硫化物的物质作为电解质。放电时，在阳极中硫基化合物中的硫-硫键被电解还原反应所裂解，从而减少了S的氧化值，充电时，由于电解氧化作用而反向形成固有的硫-硫键，提高了S的氧化值。充电时电能作为化学能储存在蓄电池内，而当放电时化学能反过来又形成电能。
锂是有效的并且因为它具有高能量密度和良好的再充电能力，所以它在有机电解质蓄电池中作为活性物质是有吸引力的。
由于锂金属能起到活性物质以及集电器的作用，所以锂阴极既可由锂金属本身制成，也以把锂金属涂覆在金属集电器基质如Cu和Ni上。因为这些金属比锂金属本身具有好得多的机械强度，所以这样的集电器经常被使用。涂覆步骤，既可以通过在集电器基质上蒸汽沉积蒸发的锂至所要求的厚度，也可以通过把锂金属箔压在另一金属箔如Cu或Ni或穿孔的集电器基质如压延金属片上而实施。
然而，蒸气沉积法昂贵且难以控制工艺过程。加压技术经常导致弱的粘附且难以控制工艺过程。另外，由于锂金属箔软，所以在加压过程中易于形成不均匀的膜。尤其是，由于锂金属与水反应性很强，特别容易与周围的水分反应而形成不希望有的氧化物或氢氧化物的表面膜。这样的表面膜影响集电器和活性物质之间紧密的粘附。另外，在锂电极表面上的这种膜还影响整个电极表面的均匀电极反应，由此破坏了蓄电池的性能与循环寿命特性。
                         发明概述
本发明的目的在于提供一种含稳定阴极的锂蓄电池，所述阴极中的锂金属是均匀地被涂覆在集电器基质上。
本发明的另一个目的在于提供一种锂蓄电池，它具有焊接到集电器基质而其中无氧化物膜的锂电极，通过简单的方法把锂金属可靠地连接到集电器上。
为了达到上述目的，本发明提供一种含锂阴电极、阳电极和置于阴电极与阳电极之间的隔板、以及渗入阴电极与阳电极以及隔板组合件的电解质的锂蓄电池。阴电极的制备，是通过在气体气氛下把锂金属熔融以制成液体锂并将该液体锂涂覆在集电器上。阳电极包括导电性金属和粘合剂以及能与锂阴电极相适应的任意阳极活性物质。阳极活性物质优选包括至少一种选自元素硫、固体Li2Sn(n≥1)以及溶于阴极电解质中的Li2Sn(n≥1)的硫基物质。电解质包括锂盐和一种有机溶剂或有机溶剂的混合物。
                    详细描述与发明
本发明的锂蓄电池使用锂金属作为阴极活性物质。锂金属具有高能量密度和良好的再充电能力。
阴电极的制备将在下面予以详细地说明。在惰性气氛下将锂金属熔融以制备液体锂。惰性气氛优选氩气且无水分和氧。假若熔融过程是在有水分和氧的气氛下进行时，则会引起锂金属和集电器基质的表面与水分和氧反应，防碍了锂在集电器基质上的紧密粘着。锂熔融过程可通过采用普通的金属熔融方法进行。代表性的是锂金属在惰性气体下在190-250℃加热以熔融锂金属，由此获得液体锂。
将液体锂按照预定厚度涂覆在金属集电器上。涂覆方法可以是任何通用的涂覆方法。优选是，用刮刀片或使用辊的压延法进行涂覆工艺，把液体金属均匀地涂覆在预热过的集电器基质的表面上。金属集电器可以是镍或铜的，或者是金属喷涂的镍或铜。金属包括锂-湿润的金属如Al、Si、Sn和其它的锂-湿润金属或合金。按照涂覆步骤，液体锂是坚固并均匀地粘着在集电器上。结果，制造出适于改进蓄电池性能的高效的锂电极。
本发明的阳极可以是任何可再充电的阳电极，它可以与锂阴电极配合。这种阳电极的优选实例是可以使用元素硫、固体Li2Sn(n≥1)和溶解于阴极电解质中的Li2Sn(n≥1)的阳极活性物质。另外，可以使用有机硫或碳-硫聚合物[(C2Sx)n，其中，X＝2.5-50，n≥2]中的至少一种。为了制备阳极，把粘合剂溶解在有机溶剂中以制备粘合剂溶剂，再把导电性物质加到溶液中并使其分散。然后，把阳极活性物质加到所获得的物质中以制成阳极活性物质浆料。再把该阳极活性物质浆料涂覆在集电器上以制备阳极。例如，作为集电器，可以使用碳涂覆的铝基质。
电导性物质包括碳、炭黑、其它导电性化合物或其混合物。粘合剂包括聚偏氟乙烯、聚四氟乙烯、聚醋酸乙烯酯、聚环氧乙烷、聚吡咯烷酮或聚乙烯醇。有机溶剂可以是相关技术中已知的任何有机溶剂，特别是丙烯腈。
电解质包括锂盐和一种有机溶剂或多种有机溶剂。有机溶剂可以是相关技术中已知的任何有机溶剂，代表性的是1，3-二氧戊环、二甘醇二甲醚、硫烷(sulforane)、二甲氧基乙烷或其混合物。锂盐可以是相关技术中已知的任何锂盐，代表性的是LiSO3CF3、lithium trflate、高氯酸锂、LiPF6或LiBF4。
下文，将参考实施例对发明进行详细地阐述。然而，这些实施例在任何情况下都不能解释为对本发明范围的限制。
                              实施例1
使金属锂在250℃下的惰性气氛(Ar)和无水分和氧的气氛中熔融以制成液体锂。将液体锂用预热过的刮刀片涂覆在预热过的Al喷涂的镍集电器上，制成具有大约250μm厚度的锂涂层的阴极。
把聚乙烯丙烯酸酯粘合剂溶解在丙烯腈溶剂中以制成粘合剂溶液。往粘合剂溶液中添加碳粉导电剂并使其分散。在此之后，把用于活性物质的、平均直径约20μm的元素硫(S8)粉末加到所获得的混合物中并用球蘑机搅拌1天，以制备阳极活性物质浆料。在此时，S8∶粘合剂∶导电剂为60∶20∶20wt％。
把所得到的浆料涂到碳涂覆的Al基质上并于80℃的干燥炉内干燥1小时。再把干燥的物质用辊压机压成50μm的厚度，以制成阳极。
阳极在真空干燥箱(60℃)内贮存1天以上，然后移入充满Ar且控制其中水分与氧含量的手套箱内。下列工艺过程在手套箱内进行。把阳极和阴极切成预定大小并把适于各阳极和阴极用的薄片附着在其中。聚乙烯的隔板放在阳极和阴极的中间。然后，在恒定的张力下把电极缠绕在一起，插入一个合中并可靠地加以密封，除了引入电解质所通过的部分。通过注入1M在1，3-二氧戊环/二甘醇二甲醚/sulforane/二甲氧基乙烷(50∶20∶10∶20体积比)中的LiSO3CF3电解质，然后密封合的未密封部分，而完成锂-硫电池的制造。
                       实施例2
借助于埋置在熔融锂槽中的导辊，让从连续辊出来的裸镍箔带通过熔融锂槽，并作为基质箔从熔融锂槽中出来，经过刮刀片控制其厚度，接着将其冷却至锂的熔点以下。结果，获得了阴极板。
借助于与实施例1相同的方法通过使用阴极板而制造锂-硫电池。
                       对比例1
除了锂箔压入镍集电器制造阴极外，按与实施例1相同的方法制造锂-硫电池。
                       对比例2
除了使用锂金属箔作锂-硫蓄电池的阴极外，按与实施例1相同的方法制造锂-硫电池。
让按照实施例1和对比例1-2的锂-硫蓄电池在0.1C下充电1小时，再于0.4C放电至1.8V。测量第一次循环的容量保留(剩余容量％)，其结果列于表1。
                                  表1
                循环
    第1次     第50次     第100次
对比例1 容量[mAh/g]     550     467     303
剩余容量[％]     100     85     55
对比例2 容量[mAh/g]     559     486     336
剩余容量[％]     100     87     60
实施例1 容量[mAh/g]     560     504     392
剩余容量[％]     100     90     70
正如从表1所见，实施例1的电池具有更好的容量而通过对比例1和2的电池充电和放电，还显示容量损失减小。
此外，按照本发明，要使锂活性物质与集电器坚固地相连，以便易于组装成电池。而且，由于锂能在集电器上涂覆均匀厚度，所以本发明能提供一种具有平稳电极反应的阴极板。
尽管已参照优选实施方案对本发明进行了详细地说明，但是，本领域的一般技术人员仍会理解在不偏离所附权利要求书所列的本发明精神和范围下可作出各种改进方案和替代方案。

Claims (12)

1.一种锂电池，包括：
通过在惰性气氛中熔融锂金属并在金属集电器上涂覆该液体锂而制备的锂阴电极；
阳极；
置于阳极与阴极之间的隔板；和
含锂盐和有机溶剂的电解质，它含于阳极和阴极以及隔板中。
2.按权利要求1所述的锂蓄电池，其中，涂覆步骤是用刮刀片进行的。
3.按权利要求1所述的锂蓄电池，其中，涂覆步骤是通过压延法进行的。
4.按权利要求1所述的锂蓄电池，其中，集电器是镍、铜或金属喷涂的镍或铜，其中金属是锂湿润的金属。
5.按权利要求4所述的锂蓄电池，其中，锂湿润的金属选自Al、Si和Sn。
6.按权利要求1所述的锂蓄电池，其中，粘合剂选自聚偏氟乙烯、聚四氟乙烯、聚醋酸乙烯酯、聚环氧乙烷、聚吡咯烷酮和聚乙烯醇。
7.一种锂-硫电池，包括：
通过在惰性气氛下熔融锂金属并在金属集电器上涂覆该液体锂而制备的锂阴极；
一种含有阳极活性物质、导电性物质和粘合剂的阳极，所述阳极活性物质含有选自元素硫和涂在集电器上的固体Li2Sn(n≥1)中的至少一种硫基物质；
置于阳极和阴极之间的隔板；和
含锂盐和有机溶剂的电解质，它含于阳极和阴极以及隔板中。
8.按权利要求7所述的锂-硫电池，其中，涂覆步骤是用刮刀片进行的。
9.按权利要求7所述的锂-硫电池，其中，涂覆步骤是通过压延法进行的。
10.按权利要求7所述的锂-硫电池，其中，集电器是镍、铜或金属喷涂的镍或铜，其中金属是锂湿润的金属。
11.按权利要求10所述的锂-硫电池，其中，锂湿润的金属选自Al、Si和Sn。
12.按权利要求7所述的锂-硫电池，其中，粘合剂选自聚偏氟乙烯、聚四氟乙烯、聚醋酸乙烯酯、聚环氧乙烷、聚吡咯烷酮和聚乙烯醇。
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