CN101563742A - 用于混合储能装置的负极 - Google Patents
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Abstract
一种用于混合储能装置的负极,其包括:集电器;紧固于集电器的至少一个面的耐腐蚀导电涂层;粘附于耐腐蚀导电涂层的包含活化碳的薄片;由负极侧面伸出的接头部;和用于包封至少一部分接头部的包含铅或铅合金的凸头。
Description
本PCT申请要求于2006年10月23日申请的美国临时申请系列No.60/853,439的优先权。
技术领域
本发明涉及一种用于混合储能装置的负极。
背景技术
混合储能装置,也已知为不对称的超级电容器或混合蓄电池/超级电容器,其合并蓄电池电极和超级电容器电极以产生具有独特特性的装置,所述特性包括循环寿命、功率密度、能量容量、快速再充电能力、以及大范围的温度可操作性。混合铅-碳储能装置使用铅-酸电池正极和超级电容器负极。参见,例如,美国专利Nos.6,466,429;6,628,504;6,706,079;7,006,346以及7,110,242。
普通的认识是,任何新的电池或超级电容器技术集合了构成成分并且使用该技术的独特工艺。此外,普通的认识是,铅-碳储能装置被要求通过对装置内部一个或多个电池采用相对高的压缩而组装起来。高度压缩是部分地由于在活化的碳活性材料和负极集电器之间存在很大的接触电阻。普通的认识还包括,通常用于制造普通铅-酸电池并且一般在汽车工业、启动动力、固定物、以及其它储能中使用的装置不能在生产混合储能装置中使用。
本发明提供了一种用于混合储能装置的负极,其能够通过使用可买到的普通铅-酸电池制造设备而被制造。本发明人已经证明,通过使用具有改进之处的普通的铅酸电池制造设备,可以制造单电池和多电池混合储能装置。可以采用铸塑设备,以与处理普通铅酸电池铅基负极相似的方式来处理活化碳基负极。
本发明的目的在于提供一种用于混合储能装置的负极,其可以通过使用容易买到的并且相对不昂贵的普通铅-酸电池制造设备而被制造。这些负极体现了改进的设计,减小了对于很大叠加压力的需要,并且获得可接受的电化学性能。因此,该负极适合于现有的铅-酸电池制造技术。
发明内容
本发明的目的在于提供一种用于混合储能装置的负极。
本发明的另一目的在于提供用于混合储能装置的负极,其能够通过使用普通的铅-酸电池制造设备而被制造。
本发明的优点是,该负极的活性材料被层叠到膨胀的石墨材料上,从而无需较高的叠加压力并且获得良好的接触电阻特性。
上述目的以及优点可以通过一种用于混合储能装置的负极而实现,该负极包括:集电器;耐腐蚀导电涂层,其紧固于集电器的至少一个面上;以及含有活化碳的片材,该活化碳粘附于耐腐蚀导电涂层并且与其电接触。接头部从集电器的侧面伸出。包含铅或铅合金的凸头包封接头部的至少一部分。
在这里使用的术语“基本上”、“通常”、“相对”、“近似”、以及“大约”是相关的修饰语,意欲表明修改后离开本质的允许的变化。其并非是意欲限于绝对值或本质性状,其虽有修改但是相当接近或者近似物理的或功能的特征。
至于术语“一个实施方式”、“实施方式”、或者“在一些实施方式中”,意思是指涉及的特征被包括在本发明的至少一个实施方式中。此外,单独谈及术语“一个实施方式”、“实施方式”、或者“在一些实施方式中”,并非必然是指相同的实施方式;然而,两者不相互排斥,除非如此表述,这对本领域技术人员而言是显而易见的。因此,本发明能够包含在本文中描述的实施方式的组合以及/或者整合的任一变化。
在下面的描述中,请参照显示用于说明可以实践本发明的具体实施方式的附图。下述说明性的实施方式被充分描述,以便本领域的技术人员能够实施本发明。应当理解,在不脱离本发明范围的情况下,基于已知的结构性等价物以及/或者功能性等价物,可以作出许多结构改变,可以使用其它实施方式。
附图说明
图1是根据本发明的实施方式的负极的剖视图。
图2是图1所示负极中的膨胀石墨薄片或箔片的示意图。
图3显示了用石蜡浸渍的膨胀石墨薄片或箔片的酸泄漏情况。
图4显示了用石蜡和松香浸渍的膨胀石墨薄片或箔片没有发生酸泄漏。
图5显示了用糠醛浸渍的膨胀石墨薄片或箔片的酸泄漏情况。
图6显示了根据现有技术的接头元件的腐蚀情况。
图7A显示了根据现有技术的接头元件上的铅锡镀层。
图7B显示了包封根据本发明的接头元件的至少一部分的凸头。
具体实施方式
图1-7B显示了根据本发明的用于混合储能装置的负极。
图1显示了根据本发明的实施方式的负极10。负极10包含集电器20。该集电器20可以是任何有效的几何形状,但优选是平整的并且呈薄片、箔片、或者网格的形态。通过具有紧固于其上的耐腐蚀导电涂层22,集电器20上至少一个面的表面的至少相当大的部分(不一定是全部)被保护起来,防止被腐蚀。
该负极还包含粘附于耐腐蚀涂层22并且与其电接触的电化学活性材料24。在特定的实施方式中,耐腐蚀导电涂层22围绕集电器20的底部被包裹。
A.集电器
集电器20含有导电材料。例如,集电器20可以包含金属材料,例如铍、青铜、含铅青铜、铜、铜合金、银、金、钛、铝、铝合金、铁、钢、镁、不锈钢、镍、其混合物、或它们的合金。优选地,集电器包含铜或铜合金。集电器20的材料可以由网格材料(例如,铜网格)做成,涂层22被压至该网格材料的表面上,以便在该集电器上得到抗腐蚀的涂层。
集电器可以包含任何电导率大于大约1.0×105西门子/m的导电材料。如果该材料显示出各向异性的导电性,那么其应当显示出沿任一方向的导电率大于大约1.0×105西门子/m。
B.耐腐蚀涂层
当存在电解质,例如,酸性电解质比如硫酸或任何其它含硫电解质时,耐腐蚀导电涂层22是化学耐性的、并且是电化学稳定的。因此,离子流向集电器或者从集电器流出被排除,同时电子传导是允许的。
耐腐蚀涂层22优选包含经浸渍的石墨材料。石墨被某一物质浸渍,从而使石墨薄片或箔片耐酸。该物质可以是非聚合性的物质,例如石蜡或糖醛。在一些实施方式中,该浸渍性物质显示出热塑性特性,并且可以具有大约25℃至大约400℃范围内的熔解温度。
优选地,石墨用石蜡及松脂浸渍。在一些实施方式中,以混合物的重量为基准,石墨可以用大约90~大约99wt%的石蜡和大约1~10wt%的松香、优选大约2~大约3wt%的松香的混合物浸渍。松香有助于石墨中的小孔被完全密封,并且因此不会被酸性电解质渗透。
石墨可以呈由高密度或低密度膨胀的石墨粒子做成的薄片或箔片的形态。优选地,出于下述原因,耐腐蚀涂层包含低密度膨胀的石墨。
从电化学活性材料24穿过耐腐蚀涂层22直至集电器20的电子传导的大部分是沿耐腐蚀涂层22的平面的法线方向。如图2所示,石墨显示出各向异性传导性。在膨胀石墨薄片中的石墨层的取向使得石墨层平面基本上与该薄片一致。
各个石墨层是具有六边形结构的碳原子的单平面薄片。高密度膨胀石墨薄片倾向于显示出比低密度膨胀石墨薄片更多的一致性。当电流被施加于高密度石墨材料的薄片或箔片时,该电流趋向形成沿与薄片或箔片平面平行的方向(即,穿过平面)的层流。因此,高密度石墨材料显示出对沿垂直于薄片或箔片的平面的方向(即,沿着平面)的电流的电阻性。
对于低密度石墨,传导性(或者电阻性)趋向为或者平行于、或者垂直于低密度石墨薄片或箔片的平面,沿两个方向大约相同。因此,因为电流必须沿垂直于集电器上的一个面或几个面的方向(即,沿着平面),所以优选使用低密度的膨胀石墨。因此,优选使用低密度膨胀石墨,以便得到较大比例的具有至少一些与膨胀石墨薄片的法线方向一致的沿平面方向的分量的石墨层,从而借此减小负极的电阻。
膨胀石墨薄片或箔片的密度范围为大约0.1至大约2.0g/cm3,优选大约0.2至大约1.8g/cm3,更优选大约0.5至大约1.5g/cm3。
在其它实施方式中,耐腐蚀涂层22可以包含含有导电材料例如炭黑的聚合物涂层。可选择地,耐腐蚀涂层22可以包含导电性的但耐腐蚀的材料,例如钛的低价氧化物或导电性金刚石材料。在一些实施方式中,钛的低价氧化物材料可以是TixO2x-1(其中x是整数),例如,Ti4O7或者Ti5O9。钛的低价氧化物更具导电性,较薄,并且可以提供比石墨更小的电阻。在一些实施方式中,导电性金刚石材料可以是通过热丝化学气相淀积(CVD)方法、微波等离子体CVD方法、等离子体电弧喷射方法、或者等离子体气相沉积(PVD)方法而沉积出的薄层或薄膜。例如,导电性金刚石中可以掺入硼。
在一些实施方式中,耐腐蚀涂层22可以包含这样一种材料:当遇到腐蚀剂(例如,强氧化剂比如硫酸)时,会形成耐腐蚀的不透酸的层。如果是硫酸,则薄层可由铅被氧化形成硫酸铅而得到。
C.电化学活性材料
负极的活性材料24包含活化碳。活化碳涉及任何主要为碳基的材料,该材料可显示出大于大约100m2/g,例如,大约100m2/g至大约2500m2/g的表面积,该表面积是通过使用普通的单点式BET技术(例如,使用Micromeritics FlowSorb III 2305/2310设备)测量的。在特定的实施方式中,活性材料可以包含活化碳、铅、以及导电性炭黑。例如,活性材料可以包含5-95wt%的活化碳;95-5wt%的铅;以及5-20wt%的导电性炭黑。
活性材料24可以呈薄片形式粘附于耐腐蚀导电性涂料22并且与其电接触。在一些实施方式中,活性材料通过利用热熔化胶而被粘附于耐腐蚀涂层。
为了使活化碳粘附于耐腐蚀导电涂层并且与其电接触,可以将活化碳粒子与合适的粘合剂物质比如PTFE或超高分子量聚乙烯(例如,分子量以百万计,通常在大约2百万和6百万之间)混合。在一些实施方式中,以活性材料及粘合剂的重量为基准,粘合剂的含量可以是大约3至大约25wt%,优选大约5至大约15wt%(例如,10wt%)。粘合剂材料优选不显示出热塑料特性或者显示出极小的热塑料特性。
活化碳以及PTFE或者超高分子量聚乙烯粘合剂将在活性材料和耐腐蚀导电涂层之间形成良好导电性所需的压力降低到小于大约5psi、优选小于大约3psi。相反,使用的聚乙烯或聚丙烯粘合剂或者用丙烯酸或丁二烯粘合剂浆料涂敷的电极要求压力大于5psi,以在活性材料和耐腐蚀导电涂层之间取得良好的接触。
D.接头部
接头部26从负极侧面伸出,例如,从集电器20伸出。在一些实施方式中,接头部是集电器的延伸。
包含铅或铅合金的凸头28被铸焊到接头部26的至少一部分、优选全部上,并且包封接头部26。可以在耐酸涂层22和活性材料24被紧固至集电器20之前涂敷凸头28,借此使这些材料免于暴露在熔铅所需的高温下。在耐腐蚀导电涂层22和活性材料24之前涂敷凸头28,还允许当紧固耐腐蚀导电涂层和活性材料时将热熔胶液41即刻涂敷至凸头28上。在一些实施方式中,该凸头通过塑模被施加于接头部。
在一些实施方式中,凸头28的厚度可以为大约0.5mm至大约10mm。选择凸头28的厚度以保证接头部26和耐腐蚀涂层22的密封不受在铸焊汇流排(COS)操作期间发生的热加工影响。根据本发明,含有铅或铅合金的铸焊汇流排30可以被铸焊到凸头28的至少一部分上。
凸头28确保集电器20不会被电解质腐蚀。在特定的实施方式中,在凸头中的铅将与硫酸电解质反应形成PbSO4,形成抗腐蚀的屏障。基于加速试验法,凸头为集电器提供了大约5年至大约10年抗腐蚀的保护。相反,使用塑料套管可以保护接头部,并且集电器容易失效,因为酸性电解质会迅速在塑料和接头部之间渗透。
实施例
实施例1:浸渍的石墨耐腐蚀涂层
制造出九个没有活性物质、但具有3种不同类型的石墨箔片(grafoil)的负极。切割指示性纸以便安装(包裹围绕)在铜集电器的两侧上。通过使用自动涂胶机械,制造出4个电极,并且用相同的胶液手工制造出5个电极。这样,如果有来自胶液的渗漏,则能够确定是否涂胶工艺有缺点或者涂胶液失败。
所有的电极用硫酸饱和,挤压进入电池壳体,然后在35psi下加压30分钟。在解除压力后,小心地冲冼电极,并且将石墨箔片从铜集电器上剥离以便研究渗漏的痕迹。
用100%石蜡浸渍的石墨箔片制造的3个电极一直在中心处有渗漏,表明没有涂胶的石墨箔片的失败,如图3所示。用98%石蜡和2%松香胶质浸渍的石墨箔片制造的3个电极都没有酸泄漏的痕迹,如图4所示。用糖醛浸渍的石墨箔片制造的2个电极没有渗漏,但是第3个电极在接近底板边缘有渗漏,并且可能是由胶剂对石墨箔片的较弱粘附引起,如图5所示。
实施例2:接头部上铅凸头
使用铅锡镀层来保护铜接头免受腐蚀,如图7A所示。铅锡材料会腐蚀并形成耐腐蚀的硫酸铅薄层。然而,铸焊汇流排工艺导致显著的涂层耗竭。在COS操作期间,接头被设置得与熔融的铅相接触。该加热的铅引起接头显著的发热,导致被拉入铅汇流排中的保护性的铅锡涂层的熔化,使得铜接头具有非常薄的保护涂层。结果是,铜接头受到硫酸电解质的腐蚀,如图6所示。
铅凸头被塑模到铜接头上,以代替铅锡镀层,如图7B所示。该铅凸头在COS操作期间不会溶化,从而维护保护性涂层。
工业实用性
一种负极,其包括:集电器;紧固于集电器的至少一个面的耐腐蚀导电涂层;粘附于耐腐蚀导电涂层的包含活化碳的薄片;以及从上述负极侧面伸出的接头部。该负极特别适用于混合储能装置。
虽然在本文中描述了本发明的具体实施方式,然而本领域的技术人员应当理解,在上述描述及示意性附图的教导下,可以对本发明的实施方式进行许多改进。
因此应当理解,本发明并不限于在本文中公开的具体实施方式,并且本发明的许多改进及其它实施方式皆应包括在本发明的范围内。此外,尽管在本文中使用了具体术语,但是它们仅仅用于普通的叙述,并不限于描述本发明。
Claims (18)
1.一种用于混合储能装置的负极,其特征在于,包括:
集电器;
紧固于所述集电器至少一个面上的耐腐蚀导电涂层;
粘附于所述耐腐蚀导电涂层的包含活化碳的薄片;
从所述负极的侧面伸出的接头部;和
将所述接头部包封起来的包含铅或铅合金的凸头。
2.如权利要求1所述的负极,其特征在于,所述薄片包含:
5-95wt%的活化碳,
5-95wt%的铅,和
5-20wt%的导电性碳。
3.如权利要求1或2所述的负极,其特征在于,所述耐腐蚀导电涂层被紧固于所述集电器的两个面上,包含活化碳的薄片被粘附于位于所述集电器两个面上的所述耐腐蚀导电涂层上并与其电接触。
4.如权利要求1或2所述的负极,其特征在于,所述集电器包含金属材料。
5.如权利要求1或2所述的负极,其特征在于,所述集电器包含电导率为1.0×105西门子/m的材料。
6.如权利要求1-4中任一项所述的负极,其特征在于,所述集电器包含铜或铜合金。
7.如权利要求1或2所述的负极,其特征在于,所述耐腐蚀导电涂层包括用石蜡和松香浸渍的膨胀石墨薄片或箔片。
8.如权利要求7所述的负极,其特征在于,所述膨胀石墨薄片或箔片包含密度范围为约0.1至约2.0g/cm3的低密度石墨。
9.如权利要求1所述的负极,其特征在于,所述集电器呈薄片、箔片、或者网格形式。
10.如权利要求9所述的负极,其特征在于,所述集电器呈网格形式,所述耐腐蚀导电涂层被压入到所述网格中。
11.如权利要求1-4中任一项所述的负极,其特征在于,所述活化碳薄片进一步包含至少一种聚四氟乙烯或者超高分子量聚乙烯。
12.如权利要求1或2所述的负极,其特征在于,所述耐腐蚀导电涂层包含由式TixO2x-1表示的钛的低价氧化物,其中x是整数。
13.如权利要求1或2所述的负极,其特征在于,所述耐腐蚀导电涂层包含导电性金刚石材料。
14.如权利要求1所述的负极,其特征在于,所述凸头的厚度为约0.05mm至约10mm。
15.一种用于混合储能装置的负极,其特征在于,包括:
集电器;
耐腐蚀导电涂层,其紧固于所述集电器的至少一个面上,并且包含用石蜡和松香浸渍的石墨薄片或箔片;
粘附于所述耐腐蚀导电涂层的包含活化碳的薄片;和
从所述负极的侧面伸出的接头部。
16.如权利要求15所述的负极,其特征在于,所述活化碳薄片进一步包含至少一种聚四氟乙烯或者超高分子量聚乙烯。
17.如权利要求15所述的负极,其特征在于,所述集电器包含铜或铜合金。
18.一种基本上如说明书附图所示的负极。
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CA (2) | CA2667300C (zh) |
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ES2498665T3 (es) * | 2006-10-23 | 2014-09-25 | Axion Power International, Inc. | Electrodo negativo para dispositivo de almacenamiento de energía híbrida |
US20080113268A1 (en) * | 2006-10-23 | 2008-05-15 | Buiel Edward R | Recombinant Hybrid Energy Storage Device |
US8202653B2 (en) * | 2006-10-23 | 2012-06-19 | Axion Power International, Inc. | Electrode with reduced resistance grid and hybrid energy storage device having same |
US20090035657A1 (en) * | 2006-10-23 | 2009-02-05 | Buiel Edward R | Electrode for Hybrid Energy Storage Device and Method of Making Same |
US7881042B2 (en) * | 2006-10-26 | 2011-02-01 | Axion Power International, Inc. | Cell assembly for an energy storage device with activated carbon electrodes |
US20090103242A1 (en) | 2007-10-19 | 2009-04-23 | Axion Power International, Inc. | Electrode with Reduced Resistance Grid and Hybrid Energy Storage Device Having Same |
CN102823037A (zh) * | 2009-12-11 | 2012-12-12 | 艾纳G2技术公司 | 含电化学改性剂的碳材料 |
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2007
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Cited By (7)
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CN102725883A (zh) * | 2009-08-27 | 2012-10-10 | 联邦科学和工业研究组织 | 电存储装置及其电极 |
CN102725883B (zh) * | 2009-08-27 | 2015-08-26 | 联邦科学和工业研究组织 | 电存储装置及其电极 |
CN101847513A (zh) * | 2010-02-26 | 2010-09-29 | 上海奥威科技开发有限公司 | 一种长寿命负极片的制备工艺及使用该负极片的电容电池 |
CN101847513B (zh) * | 2010-02-26 | 2013-08-07 | 上海奥威科技开发有限公司 | 一种长寿命负极片的制备工艺及使用该负极片的电容电池 |
CN108198695A (zh) * | 2016-12-08 | 2018-06-22 | 乾碳国际公司 | 一种混合储能装置的负极 |
CN108110222A (zh) * | 2017-12-08 | 2018-06-01 | 成都新柯力化工科技有限公司 | 一种基于锂电池的多层金属-碳负极的制备方法 |
CN108110222B (zh) * | 2017-12-08 | 2020-04-17 | 成都新柯力化工科技有限公司 | 一种基于锂电池的多层金属-碳负极的制备方法 |
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