CN101005132A - 制造用于锂/卤氧化物电化学电池的阴极集流体的装置和方法 - Google Patents
制造用于锂/卤氧化物电化学电池的阴极集流体的装置和方法 Download PDFInfo
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- CN101005132A CN101005132A CNA2006100643389A CN200610064338A CN101005132A CN 101005132 A CN101005132 A CN 101005132A CN A2006100643389 A CNA2006100643389 A CN A2006100643389A CN 200610064338 A CN200610064338 A CN 200610064338A CN 101005132 A CN101005132 A CN 101005132A
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Abstract
描述了制造用于锂/亚硫酰氯和锂/硫酰氯电池的连续的阴极集流体的装置和方法。优选的导电材料是与聚四氟乙烯(PTFE)混合的、呈干燥的粉末状的乙炔黑。所述集流体基底是镍或不锈钢箔片,该箔片被扩展成筛或者用其它方式提供冲孔。对集流体基底进行中心调整控制了其每一面上的电化学导电混合物的负载。然后,将干燥的粉末状的导电混合物连续地进料入压延机,通过在切割成样料之前使其通过集流体基底冲孔来锁定,以形成集流体结构。
Description
相关申请的交叉参考
本申请要求2005年12月22日提交的临时申请号为60/752,867的申请的优先权。
技术领域
本申请一般涉及电化学电池领域,更具体地,涉及通过新的连续进料装置制造的具有导电对集流体(counter-collector)的含锂电池。总的来说,公开了例如具有碳质化学性质的导电材料能够容易地在不脱落或者分层剥离下压制到冲孔的导电集流体基底的相对的主要面上。这就使得到的含碳的层压物特别适用作锂/卤氧化物电池中的阴极集流体。
背景技术
锂卤氧化物电池被广泛地使用于需要高重量和体积能量密度的应用中。在适用的许多尺寸和化学性质中,能够开发用于低速率或高速率应用并在低达-70℃到高达200℃的温度范围内运行的电池。阳极材料一般由锂或含有各种元素例如铝、镁或硼的锂合金构成,阴极集流体一般由某种形式的碳和适当的粘结剂一起组成。电解液一般由亚硫酰氯、磷酰氯或硫酰氯的溶剂体系组成。通常,额外的化合物或卤间化合物例如二氧化硫、氯、溴、氯化溴和其他化合物可以溶于其中以为特定的目的而改变电池例如扩大电池的运转速率或温度。还将电解质盐添加到溶剂体系中来帮助电池放电期间的离子传导。这种盐可以包括与三氯化铝或三氯化镓结合的氯化锂。然后,就地形成四氯化铝酸锂(LAC)或四氯化镓酸锂(LGC)。一般使用的阴极电解液包括具有溶于其中的LAC或LGC的氯化硫酰氯(CSC)。这些体系通常称为LAC/CSC和LGC/CSC。
元素周期表第V族或第VI族元素的液态卤氧化物是液态活性还原性阴极材料(去极化剂)。正如在本文中使用的以及在Journal of Chemical Education第49卷第587-591页(1972年9月版)中的Akiya Kozawa和R.A.Powers的题目为“Electrochemical Reactions in Batteries”中公开的,阴极去极化剂是阴极还原剂,因此,是在阴极集流体上电化学还原的材料。阴极集流体不是活性还原性材料,它作为电池的阴极端子的集流体和电子导体。换句话说,阴极集流体是活性阴极材料的电化学反应的场所和阴极端子的电子导体。
液态活性还原性阴极材料(去极化剂)可以单独地、与导电溶质混合、或与导电溶质和活性或非活性共溶剂混合用于电化学装置中(即原电池),其中导电溶剂是非活性材料但是添加其用于提高液态活性还原性阴极材料的电导率。活性共溶剂材料是电化学活性的,因此,作为活性阴极材料,而非活性共溶剂是非电化学活性的,因此,不能作为活性阴极材料。
实质上导电的任何相容的固体可用作阴极集流体。然而,期望在阴极-电解液和集流体之间具有尽可能多的表面接触,并且提供与液态阴极电解液具有高表面积界面的压制的含碳粉末集流体是优选的。这意味着制造工艺需要生产在集流板上几乎没有厚度差的具有均匀的含碳基重的集流体,所述含碳基重定义为每单位体积含碳材料的克数。当保持这些参数的精确误差时,使得电池表现为一致的放电性能。
发明内容
因此,本发明特别设计用于制造锂/亚硫酰氯和锂/硫酰氯电池用的连续的阴极集流体的设备和方法。优选的导电材料是呈干燥的粉末状的,与聚四氟乙烯(PTFE)粘结剂混合的乙炔黑。集流体基底是镍或不锈钢箔片,该基底被扩展成筛或者以其它方式提供冲孔。然后,粉末状的导电混合物连续地进料入压延机,通过在切割样料(size)之前通过集流体基底穿孔将其锁定,从而形成集流体结构。
这一工艺的关键在于进料斗组件和压延机。压延机在进料斗的正下方。进料斗包括在集流体基底的各个面上的两腔斗,一套中心引导板和振动进料系统。对进料斗组件的调整包括相对于压延间隙使集流体基底在中心,调整引导板端部到狭缝的距离,以及振动进料速度。中心调整控制了在集流体基底的各个面上的导电混合物的负载,由于基底是自定心的,该工艺可以很好地承受这一负载。通过引导板端部到压延间隙的距离控制传送到集流体基底的导电混合物的进料速率。进料斗还可以包括高和低填料传感器,该传感器调整振动系统来控制进料斗中导电混合物的重量。可以包括搅拌器以使导电混合物一贯“疏松”而没有导致不均匀涂敷的块。
通过结合附图的下述描述,本发明的这些和其他目的以及优点将变得更加明显。
附图说明
图1是根据本发明用于制造阴极集流体板的装置10的透视图。
图2是图1所示装置10的透视图,但是部分移出以示出被压延到金属集流体14上的含碳材料12。
图3是装置10的正视图。
图4是沿图3中4-4线的截面图。
图5是装置10的平面图。
图6是图4中标示区域的放大图。
图7是图1中标示区域的放大图。
图8是压延机进料斗28及其各种调整机构的详细的透视图。
具体实施方式
本装置特别适用于制造例如用于锂/卤氧化物电化学电池的压制含碳粉末集流体的阴极集流体结构。然而,更具体地,本装置可用于制造用于原电池和二次化学电池的“电极”结构。原电池的结构包括正极,正极具有担载在集流体基底上的导电或电活性材料或担载在集流体上的固态阴极活性材料的液态阴极电解液体系。
不论电池的构造如何,这种电池优选包括选自元素周期表IA、IIA或IIIB族元素的金属的阳极活性材料,包括碱金属锂、钠、钾等,以及它们的合金和金属间化合物,例如Li-Mg、Li-Si、Li-Al、Li-B、Li-Al-Mg和Li-Si-B合金及金属间化合物。优选的阳极活性材料是锂。也可使用锂合金例如锂-铝合金;然而,在合金中铝的重量百分比越大,电池的能量密度越低。
在卤氧化物或固态正极的原电池中,可以改变阳极的形式。较佳地,阳极是薄金属板或锂压制或轧制在金属阳极集流体上的箔片,例如优选包含镍。阳极集流体具有延展的接头或导线,在外壳-负极电构造中该接头或导线通过焊接接触到导电金属的电池外壳上。或者,阳极可呈一些其它的几何形状形成,例如卷筒状、圆柱形或丸状,以允许交替的低表面电池设计。
在卤氧化物电池的情况下,该电池包括担载在集流体基底上的导电材料的阴极集流体。卤氧化物电池以下列方式运行。当离子导电阴极电解液与阳极和阴极集流体可操作地结合时,在可操作地连接到阳极和阴极集流体的端子之间产生电势差。电池放电期间,在阳极上的电化学反应包括氧化反应以形成金属离子。在阴极集流体上的电化学反应包括从阳极迁移到阴极集流体的那些离子转化成原子或分子形式。另外,阴极电解液的卤素和/或卤间化合物被认为经历反应或与非水溶剂反应,因此产生化合物或络合物,该化合物或络合物展现出观察到的电池开路电压。用于阴极集流体的示例性导电材料包括与金属筛接触的乙炔黑、石墨、焦炭、炭黑和单氟化碳。由于乙炔黑的较高的锂保持容量并且因为乙炔黑含碳颗粒具有极好的机械特性以允许它们被制造成阴极集流体,因此优选的导电材料是乙炔黑。
通过干混合大约80到95重量百分比的至少一种上述限定的导电材料,优选是乙炔黑,与大约1到10重量百分比的粉末导电稀释剂和大约1到10重量百分比的粘结剂材料,优选是热塑性聚合物粘结剂材料,来制备一般的阴极集流体。术语“干”意味着导电材料和导电稀释剂的导电混合物基本上没有液体,尤其是水。
术语热塑性聚合物粘结材料是以其广义使用,并且任何聚合物材料,优选呈粉末状(该材料在电池中是惰性的并经过热塑性状态,无论最终是凝固或固化),都包含在“热塑性聚合物”的含义中。代表材料包括聚乙烯、聚丙烯和含氟聚合物例如氟化乙烯和丙烯,聚偏二氟乙烯(PVDF)、聚乙烯四氟乙烯(ETFE)和聚四氟乙烯(PTFE),后面的材料是最优选的。天然橡胶也用作本发明的粘结剂材料。
适当的导电稀释剂包括炭黑和/或石墨。优选的含碳稀释剂是KETJENBLACK碳。当与上述列出的导电材料混合时,也可使用粉末状的金属作为导电稀释剂,例如镍、铝、钛和不锈钢。然后,将这种混合物与冲孔的导电基底的至少一个主要面,优选为两个主要面接触,所述冲孔的导电基底选自镍、铜、钛、钴、钽、铝、不锈钢及其合金作为箔片或筛。导电基底优选具有大约0.001英寸到大约0.02英寸的厚度。
以下参见附图,图1到8示出了用于将导电混合物12压延到集流体基底14上的装置10。这样压延的导电结构可用作锂/卤氧化物电池的阴极集流体和锂离子电池用的含碳阳极等。装置10包括一对并排的右和左材料进料斗16和18,分别引导第一斜槽20和22,该第一斜槽20和22接着分别引导第二斜槽24和26。第二斜槽24和26将导电混合物12传送到被可调整的门30分隔的压延斗28中。与门30相连的压延斗28将导电混合物12传送到一对并排的辊32和34,辊32和34将导电混合物12压延到通过门和辊32、34移动的集流体基底14的相对的两个面上。集流体基底的移动是通过压延辊32、34的反向旋转活动进行的。
首先参考右进料斗16更加具体地描述本发明的装置10,该右进料斗16是左进料斗18的镜像结构。右进料斗16包括支撑在向下和向内成锥形的侧壁38(而不是垂直前壁40)上的上部垂直侧壁36。垂直侧壁36和前壁40环绕开口端42,导电混合物12通过开口端42载入进料斗16。锥形侧壁38汇集成斗通道部分44,该通道部分44延伸到前壁40中的出口46,通过该通道部分46导电混合物12通过重力进料到向下倾斜的第一斜槽20中。优选地,高和低填充传感器调整振动机构(用于进料斗16,未示出),所述振动机构安装在与斜槽出口46相对的锥形侧壁38的外侧,以控制进料斗中导电混合物的重量。
同样地,左进料斗18包括支撑在向下和向内成锥形的侧壁50(不是垂直前壁52)上的上部垂直侧壁48。垂直侧壁48和前壁52环绕开口端54,导电混合物12通过开口端54载入斗18。锥形侧壁50汇集成斗通道部分56,该通道部分56延伸到前壁52中的出口58,通过该通道部分56导电混合物12通过重力进料到向下倾斜的第一斜槽22中。优选地,高和低填充传感器调整振动机构60(图3),该振动机构安装在与斜槽出口58相对的锥形侧壁50的外侧,以控制进料斗18中导电混合物的重量。
用于右进料斗16的第一斜槽20是延长的通道形元件,该元件从进料斗出口46的正下方的近端延伸到远端。出口61设置在第一斜槽20的远端。那样,导电混合物12沿着第一斜槽20的长度行进并通过其出口61落到第二斜槽24中。第二斜槽24包括从底部壁66向上延伸的相对的侧壁62和64。第二斜槽侧壁62向前延伸超出了相对的斜槽侧壁64的端部。这提供了具有从侧壁62到侧壁64向内成锥形的成角度边缘68的第二斜槽底部壁66。
左进料斗18的第一斜槽22是延长的通道形元件,该元件从进料斗出口58的正下方的近端延伸到远端。出口70设置在第一斜槽72的远端。第二斜槽26还包括延长的通道形元件,该通道形元件从第一斜槽开口70正下方的近端延伸到远端。第二斜槽22包括从底部壁76向上延伸的侧壁72和74。第二斜槽侧壁74向前延伸超出了相对的斜槽侧壁72的端部。这提供了具有从侧壁74到侧壁72向内成锥形的成角度边缘78的第二斜槽部壁76。
具体地如图1到5和图8所示,并排的第二斜槽24、26将导电混合物12传输到压延机进料斗28。压延机进料斗28支撑在平台80上,包括延伸到开口84的大体是矩形的上侧壁82,通过开口84导电混合物12离开第二斜槽24、26而落下。压延机进料斗上环绕侧壁82限定了导电混合物向下移动到锥形部分86。锥形部分86包括成角度的侧壁88和90,侧壁88和90延伸到与前和后侧壁92和94相汇。成角度的侧壁88、90向下和向内延伸为具有并排辊32、34的紧密间隔的关系(图4和6)。可调整的门30将压延机进料斗28分成接受来自右第二斜槽24的导电混合物的右部分和接受来自左第二斜槽26的导电混合物12的左部分。优选地,搅拌器91设置在左和右压延机进料斗部分,以使导电混合物12一贯“疏松”,从而避免结块导致不均匀涂敷。
更详细地如图4和6所示,门30包括以垂直并排取向设置并且其间具有固定的间隙的右板96和左板98。集流体14从卷轴100展开并向下移动在门30的近端30A进入门30,通过门板96、98之间的固定间隙移动到远门端30B,然后向下并到达辊32、34之间。同时,导电混合物12沉积在压延机进料斗28中,从其前壁92到后壁94均匀地分布。这是因为各个第二斜槽24、26的向内成锥形的边缘68、78。随后,辊32以逆时针方向旋转,同时辊34以顺时针方向旋转。板96、98分别在远门端30B设置向上和外成角度的倾斜边缘96A和98A。那样,压延间隙97A和97B形成在倾斜边缘96A、98A和辊32、34各自的曲面之间。倾斜间隙97A、97B调整了压延到集流体基底14的相对的主要面上的干燥的导电混合物12的厚度。即使压制导电混合物的厚度小于压延间隙97A、97B的宽度,涂敷的厚度仍然与这些宽度直接相关。
因此,辊32、34的旋转运动拉动集流体基底14带着调整量的导电混合物12通过门板96、98,导电混合物12随后在集流体基底14的相对的主要面上压制成具有期望厚度的光滑的涂层。图4、6和7示出了包含调整的厚度的导电混合物的得到的导电结构102,所述导电混合物层压在或以其它方式涂敷在集流体基底14的相对的面上。
为了保持导电混合物以调整的厚度涂敷在集流体基底14的各个面上,装置10具有几个可调整的特征。具体如图8所示,第一可调整的机构104用于使门30在垂直方向向上和向下移动。第二可调整的机构106用于使门30在横向向后和前移动。最后,第三可调整的机构108用于使至少一个辊32、34移动来增加或减少它们之间的间隙。当示出各种可调整的机构104、106和108作为带螺纹的元件与滑块配合时,它仅是代表性的。可调整的机构104、106和108也可以是水压的、气动的或电动的来完成相同的功能。
更具体地,可调整的机构104包括固定到压延机进料斗28右侧的水平杆110。将可滑动的块112固定在压延机进料斗侧壁92的门板96、98上。该块112具有容纳带螺纹元件114的带螺纹的开口。带螺纹的元件114和滑块112之间的相对旋转移动使得滑块垂直沿进料斗侧壁92上的滑座116移动来升起或降低滑块112。接下来,导致门板96、98相对于水平轴118(图6)在向上和向下移动通过辊32、34的中心。当门30向上移动时,板96、98的倾斜边缘96A、98A和各自的辊32、34之间的压延间隙97A、97B增加,因此增加了涂敷到相对的集流体基底侧的导电混合物12的负载。相反地,当门30向下移动时,倾斜边缘96A、98A和辊之间的压延间隙97A、97B减小。这就减少了担载到相对的集流体基底主要面上的导电混合物。手柄120辅助实现带螺纹的元件114和滑块112的相对移动。距离读出器122帮助操作者精确地调整柄118。如图1到5所示,可调整的机构104具有邻近压延机进料斗侧壁94的相似的结构。
调整机构106包括固定到压延机进料斗侧壁92的门板96、98的右侧的垂直杆124。将滑块126固定在压延机进料斗侧壁92上。该块126具有容纳带螺纹的元件128的带螺纹的开口。那样,带螺纹的元件128与滑块126之间的相对旋转移动使得杆124沿水平滑座130移动。接下来,这种移动导致包括两个板96、98的门30相对于辊32、34并列前后移动。当门30朝向压延机进料斗28的成角度的侧壁88移动时,门板96的倾斜边缘96A和辊32之间的压延间隙97A减小,门板98的倾斜边缘98A和辊34之间的压延间隙98A增加。相反地,当门30朝向压延机进料斗28的成角度的侧壁90移动时,门板96的倾斜边缘96A和辊32之间的压延间隙97A增加,门板98的倾斜边缘98A和辊34之间的压延间隙97B减小了。手柄132辅助实现带螺纹的元件128和滑块124的相对移动。距离读出器134帮助操作者精确调整柄128。如图1到5所示,可调整的机构106具有邻近压延机进料斗侧壁94的相似的结构。
可调整机构108包括通过板138固定到压延机进料斗侧壁88和92上的固定杆136。转轴(axel)140支撑用于固定的旋转移动的辊32。第二板142固定地连接到压延机进料斗侧壁90和92上。横向可调整的滑块144支撑转轴(axel)146,转轴146用于其他辊34的旋转移动。空间分割销148和150连接在滑块136和板142之间。这些销148、150允许可调整的滑块144在那前后移动。通过带螺纹的元件152产生这种启动运动,该带螺纹的元件152的一端旋转地固定在可调整的滑块144上,另一端容纳在固定的第二板142的带螺纹的开口中。那样,当顺时针或逆时针转动带螺纹的元件152时,包括其转轴146和支撑辊34的可调整的滑块144前后移动朝向或离开其他辊32,以减少或增加它们之间的相对辊隙间隙。另外,调整机构108调整辊的速度,因此调整其产量。尽管在图中未示出,带有读出器的调整柄辅助操作者做出这些细小调整。类似的可调整的机构108设置在压延机进料斗28的相反侧,以均一方式调整转轴146的相反端沿着集流体基底14的宽度移动通过门30。
所得的离开压延机进料斗28的导电结构102是压制到冲孔的集流体基底14的相对的主要面的导电混合物12的层压物,它沉积到平台80上。该层压物可具有在导电基底的各个面上均匀基重,或者在相对的面上可承载不均匀基重。而且,操作者可以使用两个进料斗16、18和可调整的机构104、106和108在导电基底的相对面上担载不同的导电材料或活性材料的混合物。如前述讨论,适当的锂/卤氧化物电池用的导电活性材料包括乙炔黑、石墨、焦炭、炭黑和单氟化碳。因此,在锂/卤氧化物电池的实例中,这些材料中不同的一些,或者它们与不同负载组分的混合物可与相对的基底面接触。
在任何情况下,由于导电混合物12阻碍其本身通过集流体基底14的冲孔,因此导电结构102保持其结构完整性。而且,各种调整机构104、106和108确保了门板96、98的倾斜边缘96A、98A和辊32、34之间的压延间隙97A、97B的距离如所需的那样保持,以使导电混合物12以均匀的、调整的厚度涂敷到相对的集流体基底14的面上,并具有期望的基重,所述调整的厚度范围在大约0.020英寸到大约0.25英寸。对于电化学电池来说重要的是在建造运转中电池之间和各个建造运转之间具有一致的放电特性。然后,导电结构102可以卷绕在卷轴(未示出)上以用于以后的加工或切成适于制造工艺中的电化学电池的长度。如果需要,导电结构102还可以在后加工烧结步骤中加热至高达大约300℃。这有助于固化或凝固热塑性粘结剂以确保结构的完整性。
适于构造原电池或二次电化学电池的电极的其他导电材料选自氟化碳、金属、金属氧化物、金属硫化物或混合的金属氧化物。这些电极活性材料包括银钒氧化物、铜银钒氧化物、二氧化锰、二硫化钛、氧化铜、硫化铜、硫化铁、二硫化铁、氧化钴、氧化镍、铜钒氧化物以及通常用于碱金属电化学电池的其他材料。
适当的氟化碳由式(CFx)n和(C2F)n表示,其中x在大约0.1到1.9之间变化,优选在大约0.5到1.2之间,n指单体单元的数量,其可宽范围地变化。这些电极活性材料由碳和氟组成,包括石墨和非石墨形式的碳,例如焦炭、木炭或活性炭。
在二次电池或锂离子电池中,正极优选包括在空气中稳定并易于处理的锂化材料。这种空气稳定的锂化阴极材料的例子包括如钒、钛、铬、铜、钼、铌、铁、镍、钴和锰的金属的氧化物、硫化物、硒化物和碲化物。更优选的氧化物包括LiNiO2、LiMn2O4、LiCoO2、LiCo0.92n0.08O2和LiCo1-xNixO2。
为了使这种二次电池放电,通过施加外部产生的电势使包含锂离子的正极嵌入到含碳负极或阳极中来给电池再充电。施加的再充电势使锂离子从阴极材料中脱出,通过电解质进入含碳阳极来充满包含碳的阳极。然后,给电池提供电势并在正常模式下放电。
交替的二次电池结构包括在负极结合到电池中之前用活性锂材料嵌入含碳材料。在这种情况下,正极体可以是固态的,且包括但不限于,如二氧化锰、银钒氧化物、二硫化钛、氧化铜、硫化铜、硫化铁、二硫化铁和氟化碳的材料。然而,这种方法产生处理电池外的锂化碳的问题。当与空气或水接触时,锂化碳易于反应。
原电池或二次电池的正极以前述的卤氧化物电池阴极集流体的制备相似的方式制备。在这方面,通过混合大约80到99重量百分比的已经制备好的细分离的导电材料与大约1到10重量百分比的粉末导电稀释剂和大约1到10重量百分比的粘结剂材料来制备正极。适当的导电稀释剂和粘结剂材料已经描述过了。
相似地,如果所述活性材料是在二次电池中的含碳对电极,电极材料优选包括导电稀释剂和粘结剂材料,与之前描述的原电池、固态阴极电化学电池相似。
如上述方法制备的电极是挠性的,可以一个或多个板的形式可操作地与至少一个或多个对电极材料的板结合,或在类似“果冻卷”的结构中以条形与相应的对电极材料条卷绕。
对于卤氧化物电化学电池,它还包括可操作地与阳极和阴极集流体结合的非水、离子导电阴极电解液。在具有固态正极的电池化学电池中,用离子导电电解液活化阳极和阴极。在任一情况下,阴极电解液和电解液作为(在卤氧化物化学电池的情况下)阳极和阴极集流体之间的离子迁移的媒介,以及电池的电化学反应期间固态正极化学电池的阳极和阴极之间的离子迁移的媒介。
对于卤氧化物电池,适当的非水溶剂去极化剂表现出离子传导所需的物理特性,即低粘度、低表面张力和润湿性。当是阴极电解液时,适当的非水去极化剂由溶于非水共去极化剂体系中的无机盐,更优选的是溶于含溶于非水溶剂的卤素和/或卤间化合物的阴极电解液中的锂金属盐构成。卤素和/或卤间化合物作为可溶的去极化剂。它们也可以在电化学电池中作为共溶剂。卤素选自碘、溴、氯或氟组成的组,同时卤间化合物选自ClF、ClF3、ICl、ICl3、IBr、IF3、IF5、BrCl、BrF、BrF3、BrF5及其混合物。溶于上述非水有机或无机溶剂中任一种的上述卤素和/或卤间化合物中的任一种的摩尔比在大约1∶6到大约1∶1的范围。
非水溶剂去极化剂可以是对阳极和导电集流体材料基本上是惰性的有机溶剂的一种,例如四氢呋喃、碳酸丙烯酯、乙腈、二甲基亚砜、二甲基甲酰胺、二甲基乙酰胺,具体是卤代的有机溶剂例如1,1,1,2,3,3,3-七氯丙烷或1,4二氟八氯丁烷。所述非水溶剂去极化剂还可以是有机溶剂的一种或多种的混合物,可用作溶剂和去极化剂例如亚硫酰氯,硫酰氯、二氯氧化硒、氯化铬酰、磷酰氯、三氯磷硫等。非水阴极电解液的离子导电性优选通过将锂盐溶于非水去极化剂中来制备。锂盐的实例是卤化锂例如LiCl和LiBr,和LiMXn型锂盐,例如LiPF6、LiBF4、LiAsF6、LiSbF6、LiClO4、LiAlCl4、LiGaCl4、LiC(SO2CF3)3、LiN(SO2CF3)2、LiSCN、LiO3SCF2CF3、LiC6F5SO3、LiO2、LiO2CCF3、LiSO3F、LiB(C6H5)4、LiCF3SO3及其混合物。适当的锂盐浓度通常在大约0.25到大约1.5摩尔的范围。因此,卤素和/或卤间化合物溶液、非水溶剂去极化剂、以及任选地,离子盐用作卤氧化物电池的共去极化剂和阴极电解液。
在具有固态阴极和固态正极的原电池或二次化学电池的电化学系统中,非水溶剂体系包括含四氢呋喃(THF)、乙酸甲酯(MA)、二甘醇二甲醚、三甘醇二甲醚、四甘醇二甲醚、碳酸二甲酯(DMC)、碳酸乙基甲酯(EMC)、1,2-二甲氧基乙烷(DME)、二异丙基醚、1,2-二乙氧基乙烷、1-乙氧基、2-甲氧基乙烷、碳酸二丙酯、碳酸乙基甲酯、碳酸甲基丙酯、碳酸乙基丙酯、碳酸二乙酯及其混合物的低粘度溶剂。然而不是必需的,所述电解液也可以优选地包括选自环状碳酸酯、环状酯和环状酰胺例如碳酸丙烯酯(PC)、碳酸乙烯酯(EC)、碳酸丁烯酯、乙腈、二甲基亚砜、二甲基甲酰胺、二甲基乙酰胺、γ-丁内酯(GBL)、γ-戊内酯、N-甲基吡咯烷酮(NMP)及其混合物的高介电常数的溶剂。所述非水溶剂体系还包括上述锂盐中的至少一种,浓度为大约0.8到大约1.5摩尔。对于具有锂作为阳极活性材料的固态阴极原电池或二次电池,例如Li/SVO电对,优选的电解液是LiAsF6,溶于50∶50体积比的PC/DME混合物中。对于Li/CFx电池,优选的电解液是1.0M到1.4M的LiBF4,溶于γ-丁内酯(GBL)中。
当所述电池的机械结构或构造需要时,使用隔膜提供卤氧化物电池用阳极和阴极集流体之间以及固态正极化学电池中阳极和阴极之间的物理隔离。所述隔膜是电绝缘性材料,且隔膜材料还是与对电极材料不发生化学反应,并且不与阴极电解液或电解液反应也不溶于其中(视需要)。另外,所述隔膜材料的孔隙度足以在电池的电化学反应期间使阴极电解液或电解液流过。
示例的隔膜材料包括用多烯烃或含氟聚合物多孔膜层压或叠置的多烯烃纤维或含氟聚合物纤维的纺织和无纺织物,该含氟聚合物纤维包括聚乙烯四氟乙烯、聚偏二氟乙烯和聚乙烯氯三氟乙烯。适当的多孔膜包括市售的标识为ZITEX(Chemplast Inc.)的聚四氟乙烯膜、市售的标识为CELGARD(Celanese PlasticCompany,Inc.)的聚丙烯膜和市售的标识为DEXIGLAS(C.H.Dexter,Div.,Dexter Corp.)的膜。隔膜还可以由无纺玻璃、玻璃纤维材料和陶瓷材料组成。
隔膜的形式通常是板状,该隔膜插在阳极和阴极集流体之间或负极和正极之间,起到防止它们之间物理接触的作用。当在类似螺旋形结构中阳极被折叠(在该结构中,多个阴极集流体板或正极板设置在折叠的阳极之中并容纳于电池壳中)时,或当辊轧电极组合或以其他方式形成为圆柱形的“果冻卷”结构时,情况是这样的。
本文中描述的电池组件优选呈卷绕的单元电池的形式。即,制得的阴极集流体或正极、阳极或负极集流体和隔膜卷绕在一起成“果冻卷”型结构或“卷绕单元电池堆”,使得阳极或负极位于卷的外侧,从而与在壳-负极结构中电池壳电接触。使用适当的顶部和底部绝缘体,将卷绕电池堆插入适当尺寸的金属外壳中。金属外壳可以包括金属例如不锈钢、低碳钢、镀镍低碳钢、钛、钽或铝,但不限于此,只要所述金属材料适于用作电池的元件。
电池帽包括带有第一孔和第二孔的金属圆盘体,其中,第一孔用于容纳玻璃-金属密封/终端引线接头,第二孔用于电解液填充。使用的玻璃是具有高达约50重量%的硅例如CABAL12、TA 23、FUSITE 425或FUSITE 435的耐腐蚀型玻璃。尽管也可以使用钼、铝、镍合金或不锈钢,但是阴极集流体或正极终端引线接头优选包括钛。所述电池帽包括与电化学电池的其他元件相容并且抗腐蚀的元件。阴极集流体或正极引线焊接到玻璃-金属密闭中的正极引线接头上,帽焊接到含有电极堆的外壳上。然后,如上述用阴极电解液或电解液填充电池,密封例如将不锈钢球密闭焊接到填充孔中,但不限于此。
上述组件描述了外壳-负极电池,它是本发明的示例的化学电池的优选的结构。本领域技术人员可以理解,示例的电化学体系还可以构建成外壳-正极结构。
在不偏离所附权利要求书中限定的本发明的范围的前提下,对本文中描述的发明概念进行各种修改对于本领域技术人员而言是显而易见的。
Claims (40)
1、一种将导电材料与集流体基底接触的装置,该装置包括:
a)含有导电材料的压延机进料斗,包括出口,所述导电材料通过出口移动;
b)设置在所述压延机进料斗出口的一对并排的第一和第二反向旋转的压延辊;
c)将进料斗分割为在第一和第二压延辊正上方的第一部分和第二部分空间的门,其中,所述门包括容纳集流体基底引导端的近门端和位于所述第一和第二辊的辊隙上方的远门端;以及
d)所述集流体基底可通过第一和第二辊的反向旋转移动通过门从近门端移动到远门端,所述第一和第二辊通过调整远门端与第一和第二辊之间的压延距离接触具有与所述集流体基底的主要面接触的调节量的导电材料的辊的辊隙处的集流体基底的相对的主要面。
2、根据权利要求1的装置,它还包括进料斗,所述进料斗起初包含导电材料并包含通向斜槽的出口,该斜槽容纳导电材料并将其移送到压延机进料斗。
3、根据权利要求2的装置,其特征在于,所述进料斗包括用于帮助导电材料移动到斜槽的振动机构。
4、根据权利要求1的装置,其特征在于,该门平分压延机进料斗,且相对于通过第一和第二辊的各个旋转轴和它们之间的辊隙的轴呈垂直取向。
5、根据权利要求1的装置,其特征在于,该门包括第一和第二并排板,在两板之间所述集流体基底从近门端移向远门端。
6、根据权利要求5的装置,其特征在于,所述第一和第二门板在它们的远端分别向上和向外倾斜。
7、根据权利要求1的装置,其特征在于,该门可相对于第一和第二辊之间的压延距离向上和向外调整。
8、根据权利要求1的装置,其特征在于,该门可面向和离开所述第一或第二辊横向调整。
9、根据权利要求1的装置,其特征在于,所述第一和第二辊之间的辊隙是可调整的。
10、根据权利要求1的装置,其特征在于,所述进料斗的出口接近第一和第二辊的斜槽曲面。
11、根据权利要求1的装置,其特征在于,所述导电材料是基本上干燥的。
12、根据权利要求1的装置,其特征在于,所述导电材料选自乙炔黑、石墨、焦炭、炭黑、单氟化碳及其混合物。
13、根据权利要求1的装置,其特征在于,所述导电材料包括导电稀释剂。
14、根据权利要求13的装置,其特征在于,所述导电稀释剂选自热塑性聚合物、天然橡胶和金属粉末。
15、根据权利要求2的装置,其特征在于,所述进料斗包括第一和第二进料斗,用于将导电材料分别供给到所述压延机进料斗的第一和第二部分。
16、根据权利要求2的装置,其特征在于,所述第一和第二进料斗通向各个具有成角度的远端边缘的斜槽,所述斜槽均匀地分配导电材料通过导电基底的相对的主要面的宽度。
17、根据权利要求2的装置,其特征在于,所述第一和第二进料斗容纳不同的导电材料。
18、根据权利要求2的装置,其特征在于,所述第一和第二进料斗以不同的负载容纳两种或者多种导电材料的混合物。
19、根据权利要求2的装置,其特征在于,所述第一和第二进料斗以不同的负载容纳至少一种导电材料和至少一种导电稀释剂。
20、根据权利要求2的装置,其特征在于,所述进料斗包括用于调整包含于其中的导电材料的含量的传感器。
21、根据权利要求1的装置,其特征在于,所述压延机进料斗包括用于保持导电材料呈疏松状态的搅拌器。
22、根据权利要求1的装置,其特征在于,所述集流体基底是选自镍、铜、钛、钴、钽、铝、不锈钢及其合金作为箔片或筛的冲孔结构。
23、根据权利要求1的装置,其特征在于,所述导电材料以不同的厚度位于导电基底的相对的主要面上。
24、一种使导电材料与集流体基底接触的装置,该装置包括:
a)第一和第二进料斗,它起始含有导电材料,各个进料斗都包括出口;
b)第一和第二斜槽,它接收来自所述第一和第二进料斗的出口的导电材料,并具有成角度的远斜槽边缘;
c)压延机进料斗,它接收来自所述第一和第二斜槽的导电材料,所述压延机进料斗包括出口,所述导电材料可通过该出口移动;
d)设置在所述压延机进料斗出口的一对并排的第一和第二反向旋转的压延辊;
e)将进料斗分割为在第一和第二压延辊正上方的第一部分和第二部分空间的门,其中,该门包括容纳所述集流体基底的引导端的近门端以及位于所述第一和第二辊的辊隙之上的远门端,第一和第二斜槽的成角度的远端均匀地分配导电材料进入进料斗并通过所述导电基底的相对的主要面的宽度;以及
f)所述集流体基底可通过所述第一和第二辊的反向旋转移动通过门从近门端移向远门端,所述第一和第二辊通过调整远门端与第一和第二辊之间的压延距离在具有调节量的接触集流体基底的主要面的导电材料的辊的辊隙处与集流体基底的相对的主要面接触。
25、根据权利要求24的装置,其特征在于,该门平分压延机进料斗,且相对于通过所述第一和第二辊的各个旋转轴和它们之间的辊隙的轴呈垂直取向。
26、根据权利要求24的装置,其特征在于,该门包括第一和第二并排板,在两板之间所述集流体基底从近门端移向远门端。
27、根据权利要求26的装置,其特征在于,所述第一和第二门板在它们的远端分别向上和向外倾斜。
28、根据权利要求24的装置,其特征在于,该门可相对于所述第一和第二辊之间的压延距离向上和向外调整。
29、根据权利要求24的装置,其特征在于,该门可面向和离开所述第一或第二辊横向调整。
30、根据权利要求24的装置,其特征在于,所述第一和第二辊之间的辊隙是可调整的。
31、根据权利要求24的装置,其特征在于,所述导电材料是基本上干燥的。
32、根据权利要求24的装置,其特征在于,所述导电材料选自乙炔黑、石墨、焦炭、炭黑、单氟化碳及其混合物。
33、根据权利要求24的装置,其特征在于,所述导电材料包括导电稀释剂。
34、根据权利要求24的装置,其特征在于,所述第一和第二进料斗容纳不同的导电材料。
35、根据权利要求24的装置,其特征在于,所述第一和第二进料斗以不同的负载容纳两种或者多种导电材料的混合物。
36、根据权利要求24的装置,其特征在于,所述第一和第二进料斗以不同的负载容纳至少一种导电材料和至少一种导电稀释剂。
37、根据权利要求24的装置,其特征在于,所述导电材料以不同的厚度位于所述导电基底的相对的主要面上。
38、一种提供电化学电池的方法,包括以下步骤:
a)提供将导电材料与集流体基底接触的装置,该装置包括:
i)压延机进料斗,它含有导电材料并包括出口,所述导电材料可通过该出口移动;
ii)设置在所述压延机进料斗出口的一对并排的第一和第二反向旋转的压延辊;
iii)将所述进料斗分割为在第一和第二压延辊正上方的第一部分和第二部分空间的门,其中,该门包括近门端和位于所述第一和第二辊的辊隙之上的远门端;
b)通过所述第一和第二辊的反向旋转移动将集流体基底通过门从近门端移向远门端,该第一和第二辊在所述辊的辊隙处与集流体基底的相对的主要面接触;
c)通过调整所述远门端与所述第一和第二辊之间的压延距离调整接触所述集流体基底的主要面的导电材料的量,从而提供导电结构;
d)在导电结构和对电极之间设置隔膜,从而提供电极组件;以及
e)将所述电极组件装入到用电解液活化的外壳中。
39、根据权利要求38的方法,包括提供导电结构和在锂卤氧化物电池中或作为锂离子电池阳极的阴极集流体。
40、根据权利要求38的方法,包括从由乙炔黑、石墨、焦炭、炭黑、单氟化碳、银钒氧化物、铜银钒氧化物、二氧化锰、二硫化钛、氧化铜、硫化铜、硫化铁、二硫化铁、氧化钴、氧化镍、铜钒氧化物、锂钴镍氧化物、LiNiO2、LiMn2O4、LiCoO2、LiCo0.92Sn0.08O2及其混合物中选择导电材料。
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