CN104081572B - 固体高分子燃料电池用膜电极接合体 - Google Patents
固体高分子燃料电池用膜电极接合体 Download PDFInfo
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- CN104081572B CN104081572B CN201380007726.1A CN201380007726A CN104081572B CN 104081572 B CN104081572 B CN 104081572B CN 201380007726 A CN201380007726 A CN 201380007726A CN 104081572 B CN104081572 B CN 104081572B
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- Sustainable Energy (AREA)
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- Fuel Cell (AREA)
- Inert Electrodes (AREA)
Abstract
在于气体扩散层(12a)和(12b)之间夹持两面具备催化剂层(11a、11b)的高分子电解质膜(10)并用第一塑料薄膜(13)覆盖其外周缘部而成的层叠体的表面整面和背面整面配置金属多孔体(14a、14b),进一步用第二塑料薄膜(15)覆盖所叠合的上述层叠体和金属多孔体(14a、14b)的外周缘部。
Description
技术领域
本发明涉及作为固体高分子燃料电池(PEFC)的发电元件使用的膜电极接合体以及使用了该膜电极接合体的固体高分子燃料电池。
背景技术
使用了质子传导性固体高分子膜的固体高分子燃料电池与固体氧化物燃料电池、熔融碳酸盐燃料电池之类的其他类型的燃料电池相比,在低温(常温)工作,因此作为汽车等移动物体用的动力源,其实用化也在推进。
这种固体高分子燃料电池(以下有时简记为“PEFC”)一般采用将发挥发电功能的多个单电池层叠得到的结构。
该单电池分别具备膜电极接合体(MEA:Membrane Electorode Assembly),所述膜电极接合体包括具有质子传导性的高分子电解质膜(例如Nafion(注册商标)膜)、夹持该电解质膜的1对阳极、阴极的电极层(也称为“电极催化剂层”)、以及夹持这些电解质膜和电极层的1对阳极、阴极的气体扩散层。另外,作为上述气体扩散层(以下有时简记为“GDL”),一般可使用碳纸、碳布等。
将构成单个单电池的膜电极接合体(以下有时简记为“MEA”)与隔着隔离体邻接的单电池的MEA电连接,如此将单电池层叠、连接,由此构成燃料电池堆。而且,这种燃料电池堆适用于各种用途,作为发电手段发挥功能。
对于这种膜电极接合体,已知有各种结构的膜电极接合体,但上述高分子电解质膜在本质上缺乏强度,为了防止在受到由燃料气体与氧化剂气体的压力差、周边构件的热应变等引起的应力时破损、由此导致的气体混合(交叉泄漏)而提出了各种方案。例如,专利文献1中公开了:为了弥补未配置电极(气体扩散电极)的固体高分子电解质膜的外缘部的强度不足,而用由氟树脂、聚丙烯等构成的增强膜被覆电极外周缘部和电解质膜的外缘部。
现有技术文献
专利文献
专利文献1:日本特许第3052536号公报
发明内容
发明要解决的问题
然而,在上述文献记载的发明中,即使能够增强自电解质膜的电极露出的露出部分、即MEA中强度上最弱的部分,也无法提高MEA自身的强度、刚性,在过剩的应力作用于MEA整体时,存在电解质膜会发生破损的问题。
本发明是为了解决现有固体高分子燃料电池中的这种问题而做出的,其目标的在于提供强度、刚性优异而不会伴随厚度的增加、气体扩散层的透气性劣化的膜电极接合体,以及具备这种膜电极接合体的固体高分子燃料电池。
用于解决问题的方案
本发明人等为了实现上述目的而进行了各种研究,结果发现,通过在MEA的表面整面和背面整面配置作为GDL的一部分发挥功能的金属多孔体并利用塑料薄膜覆盖其外周缘部,能够实现上述目的,从而完成了本发明。
本发明是基于上述认识做出的,本发明的固体高分子燃料电池用膜电极接合体的特征在于是如下得到的,在于气体扩散层之间夹持两面具备催化剂层的高分子电解质膜并用第一塑料薄膜覆盖其外周缘部而成的层叠体的表面整面和背面整面配置金属多孔体,进一步用第二塑料薄膜覆盖所叠合的上述层叠体和金属多孔体的外周缘部。
此外,本发明的固体高分子燃料电池的特征在于应用了本发明的上述膜电极接合体。
发明的效果
根据本发明,在夹持了两面具备催化剂层的高分子电解质膜的气体扩散层的表面分别配置以例如金属丝网等为代表的金属多孔体,用塑料薄膜覆盖 其外周缘部,因此能够提高膜电极接合体的强度和刚性,抑制由应力负载导致的变形,防止破损。
附图说明
图1是对将本发明的燃料电池层叠而成的燃料电池堆进行说明的分解状态的立体图(A)和示出组装后的立体图(B)。
图2是对本发明的燃料电池的一个实施方式进行说明的分解状态的俯视图(A)和示出组装后的俯视图(B)。
图3是示出本发明的固体高分子燃料电池用膜电极接合体的结构的主要部分剖视图。
具体实施方式
以下,对于本发明的固体高分子燃料电池用膜电极接合体,基于附图进一步具体说明其实施方式。
图1和图2所示的燃料电池(也称为单电池)C层叠多片,构成图1所示的燃料电池堆FS。
燃料电池堆FS如图1的(A)所示,相对着燃料电池C的层叠体S,在层叠方向的一个端部(图1中为右侧端部)隔着集电板54A和间隔物55设置有端板56A,并且在另一端部隔着集电板54B设置有端板56B。此外,对于燃料电池堆FS,相对着层叠体S,在作为单电池C的长边侧的两面(图1中为上下面)设置有固定板57A、57B,并且在作为短边侧的两面设置有增强板58A、58B。
接着,燃料电池堆FS通过螺栓B将各固定板57A、57B和增强板58A、58B与两端板56A、56B连接。如此,燃料电池堆FS形成如图1的(B)所示的壳一体型结构,对层叠体A在其层叠方向上进行约束并加压,对单个单电池C施加规定的接触面压力,良好地维持气体密封性、导电性等。
燃料电池C如图2所示,具备在周围具有框51的膜电极接合体1、以及在框51与膜电极接合体1之间形成阴极和阳极的气体流路(GC、GA)的一对 隔离体2、2。而且,燃料电池C形成为使两气体流路(GC,GA)中的气体的流动方向互为反方向的结构。
膜电极接合体1一般具有用1对电极层夹持了由固体高分子构成的电解质层10的结构。一侧的电极层具有与电解质层10接触的电极催化剂层11a以及配置在其外侧的气体扩散层(GDL)12a,另一侧的电极层也同样具有电极催化剂层11b以及气体扩散层12b(参见图3)。
框51通过树脂成形(例如注塑成形)而与膜电极接合体1一体化,该实施方式中,使膜电极接合体1位于中央并呈长方形。此外,框51在短边两侧分别各排列有三列歧管孔,从各歧管孔组到膜电极接合体1的区域为扩散部D。该框51和两隔离体2、2均为具有基本相同的长宽尺寸的长方形。
进而,框51如图2所示,在扩散部D纵横排列有圆形的多个突部52。这些突部52在膜电极接合体1随时间变化等而在单电池C中产生厚度方向的变形时与隔离体2、2接触,维持反应用气体的流通空间。
各隔离体2为具有表面背面反转形状的金属制的板构件,例如不锈钢制,可以通过压制加工而成形为适当形状。图示例的隔离体2至少在与膜电极接合体1对应的中央部分形成有截面凹凸形状。该隔离体2在长边方向连续具有截面凹凸形状,使波形凸部与膜电极接合体1接触,并且通过波形凹部在与膜电极接合体1之间形成阴极和阳极的气体流路(GC、GA)。此外,各隔离体2在两端部具有与框51的各歧管孔相同的歧管孔。
上述框51以及膜电极接合体1和两隔离体2、2叠合构成燃料电池C。此时,单电池C特别如图2的(B)所示,在中央具备为膜电极接合体1的区域的发电区域G。此外,在发电区域G的两侧具备用于供给和排出反应用气体的歧管部M以及作为从各歧管部M到发电部G的反应用气体的流通区域的扩散部D。
在图2的(B)的左侧所示的一侧的歧管部M中,各歧管孔从上侧起为阳极气体供给用(AI)、冷却流体排出用(FO)和阴极气体排出用(CO),沿层叠方向相互连通而形成各自的流路。此外,在图2的(B)的右侧所示的另 一侧的歧管部M,各歧管孔从上侧起为阴极气体供给用(CI)、冷却流体供给用(FI)和阳极气体排出用(AO),沿层叠方向相互连通而形成各自的流路。
进而,燃料电池C如图2所示,在框51的缘部与各隔离体2的缘部之间、在歧管孔的周围E设置有气封SL。此外,在将多个燃料电池C层叠了的状态下,在燃料电池C之间即邻接的隔离体2与隔离体2之间也设置气封SL。在歧管孔的外周缘部的合适位置设置开口,以使该气封SL在各个层间将阴极气体、阳极气体和冷却液各自的流通区域气密性地分离,并且使规定的流体在其层间流动。
具备上述构成的燃料电池C向膜电极接合体1的一侧的电极层供给阴极气体(含氧气体/空气),并且向另一侧的电极层供给阳极气体(含氢气体),由此通过电气化学反应进行发电。
即,燃料电池C在阳极电极侧,在阳极电极催化剂层中,由阳极催化剂使氢(H2)反应而形成质子(2H+)。该质子(2H+)与水(H2O)一起经由电解质层10向阴极侧移动。此外,在阴极电极侧,由阴极催化剂使质子(2H+)与氧(O2)反应而生成水(H2O)。进而,在阴极电极生成的水(H2O)的一部分经由电解质层10向阳极电极侧移动。
图3是示出本发明的固体高分子燃料电池用膜电极接合体的结构的、主要部分的剖视图。
图示的膜电极接合体(MEA)1在中心部具有两面具备催化剂层11a和11b的高分子电解质膜10、即催化剂被覆膜(CCM:Catalyst Coated Membrane),该CCM被1对气体扩散层(GDL)12a和12b夹持。
接着,在夹持了上述CCM的状态的GDL 12a和12b的外周缘部安装有第一塑料薄膜13,可以利用其覆盖、密封CCM和GDL 12a、12b的端缘部。
上述高分子电解质膜10具有使PEFC运行时在阳极电极层生成的质子朝向阴极电极层沿膜厚方向选择性透过的功能,此外,还具有作为用于不使供给阳极侧的燃料气体与供给阴极侧的氧化剂气体混合的隔壁的功能。
作为这种高分子电解质膜,除了一般使用的全氟磺酸类电解质膜以外,还可以使用烃类电解质膜。
作为全氟磺酸类电解质膜,例如可列举出:Nafion(注册商标、杜邦公司制造)、Aciplex(注册商标、旭化成株式会社制造)、Flemion(注册商标、旭硝子株式会社制造)等全氟碳磺酸类聚合物、全氟碳膦酸类聚合物、三氟苯乙烯磺酸类聚合物、乙烯-四氟乙烯-g-苯乙烯磺酸类聚合物、乙烯-四氟乙烯共聚物、聚偏二氟乙烯-全氟碳磺酸类聚合物等。
而作为烃类高分子电解质,例如可列举出:磺化聚醚砜(S-PES)、磺化聚芳基醚酮、磺化聚苯并咪唑烷基、膦酸化聚苯并咪唑烷基、磺化聚苯乙烯、磺化聚醚醚酮(S-PEEK)、磺化聚亚苯基(S-PPP)等。
对于高分子电解质膜10的厚度,考虑所得燃料电池的特性来适当决定即可,并没有特别限制,通常为5~300μm左右。只要高分子电解质膜的厚度在这种数值范围内,则制膜时的强度、使用时的耐久性和使用时的输出特性之间取得合适的平衡。
作为催化剂层11a、11b,在负载有催化剂成分的导电性的催化剂载体中混入全氟磺酸类电解质溶液、烃类电解质溶液而形成。另外,也可以根据需要而添加拒水剂、增孔剂。
作为催化剂成分的具体例子,可列举出:铂(Pt)、钌(Ru)、铱(Ir)、铑(Rh)、钯(Pd)、锇(Os)、钨(W)、铅(Pb)、铁(Fe)、铬(Cr)、钴(Co)、镍(Ni)、锰(Mn)、钒(V)、钼(Mo)、镓(Ga)、铝(Al)等金属、它们的合金等。
这些当中,为了提高催化剂活性、相对于一氧化碳等的耐中毒性、耐热性等,适宜使用至少含有铂的成分。作为这种合金的组成,虽然也取决于进行合金化的金属的种类,但优选使铂的含量为30~90原子%。
另一方面,作为催化剂载体,只要具有用于以所期望的分散状态负载催化剂成分的比表面积、具有充分的电子传导性即可,具体可列举出:油炉法炭黑、乙炔黑、热炭黑(thermal black)、槽法炭黑等炭黑,活性炭、焦炭、天然石墨、人造石墨等的碳颗粒。
气体扩散层12a、12b具有促进通过在与未图示的隔离体之间形成的气体流路(燃料气体流路、氧化剂气体流路)所分别供给的燃料气体、氧化剂气体向电极层扩散的功能,并且具有作为电子传导路径的功能,由碳纸、碳布等碳材料构成。
另外,上述气体扩散层也可以应用微孔层。
微孔层(MPL:Micro Porous Layer)是指以聚四氟乙烯(PTFE)等拒水性树脂和炭黑等导电性材料为主要成分的涂布层。
而且,通过使GDL整体为这种微孔层,或者通过使其电解质膜侧为微孔层,使得其具备将水分保持在电解质膜中或将MEA中多余的水分排出而抑制液泛(flooding)的功能。
作为用于密封上述CCM和GDL 12a、12b的周端缘部的塑料薄膜13,只要具有针对燃料气体、氧化剂气体的不透过性,则对其材料没有特别限定,可以使用公知的材料。
作为这种树脂材料,例如可列举出:聚萘二甲酸乙二醇酯(PEN)、聚对苯二甲酸乙二醇酯(PET)、聚四氟乙烯(PTFE)、聚偏氟乙烯(PVDF)等。
接着,对于处于将CCM(电解质膜10、催化剂层11a、11b)与GDL 12a、12b叠合并进一步用塑料薄膜13覆盖其外周缘部的状态的层叠体,分别在其表面整面和背面整面配置金属多孔体14a和14b。
接着,在重叠于层叠体的两面的金属多孔体14a、14b的外周缘部安装由上述同样的材料构成的第二塑料薄膜15,与之前安装的第一塑料薄膜13一起覆盖上述金属多孔体14a、14b的端缘部进行密封。
另外,在基于图3所示的实施方式的膜电极接合体中,作为上述金属多孔体14a、14b,示出了使用金属丝网的例子。然而,作为上述金属多孔体,并不一定限定于此,除了金属丝网以外,还可以使用例如发泡金属、金属板网(expand metal)、冲孔金属、蚀刻板、精密压制加工板、金属网、金属细 线烧结体、金属无纺布等。
此外,在安装上述塑料薄膜13、15时,可以应用热压接等,而根据材料的种类,也可以为了提高塑料薄膜之间或者与GDL、金属多孔体的密合性而在它们之间设置由热可塑性树脂等构成的粘接层16。此外,也可以出于同样的目的而使用带粘接剂的薄膜、例如层压片等作为塑料薄膜。
对于上述膜电极接合体1,将多个膜电极接合体固定为隔着具备燃料气体和氧化剂气体的流路的隔离体层叠的状态从而形成燃料电池堆,将其装入合适的壳内,由此构成固体高分子燃料电池。
接着,在这种膜电极接合体1中,由于分别在GDL 12a和12b的表面配置有气体透过性优异的金属多孔体14a和14b,因此一起作为气体扩散层的一部分发挥功能,无需增加厚度即可以提高气体扩散层的强度。因此,刚性优异的膜电极接合体1即使应力负荷增加,其变形也小,可以抑制膜电极接合体1、特别是电解质膜10的破损,提高耐用寿命。
此外,由于上述金属多孔体14a、14b的端缘部被第二塑料薄膜15覆盖,可以防止由自端部的腐蚀导致的性能劣化,并且可以防止金属多孔体端部绽开,可以防止由绽开的单丝(特别是金属丝网的情况下)导致的短路。
此外,由于金属多孔体14a、14b是在用第一塑料薄膜13覆盖CCM(电解质膜10、催化剂层11a、11b)与GDL 12a、12b的层叠体的外周缘部的状态下装入,因此可以防止因绽开的单丝陷入CCM、GDL而导致的短路、电解质膜10的破损(开孔)。
以上对本发明的固体高分子燃料电池用膜电极接合体的实施方式例进行了说明,但本发明的膜电极接合体并不仅仅限于上述实施方式,可以在不脱离本发明的思想的范围内对构成的细部进行适当变更,这是不言而喻的。
附图标记说明
1 固体高分子燃料电池用膜电极接合体(MEA)
10 高分子电解质膜
11 催化剂层
11a、11b 催化剂层
12a、12b 气体扩散层(GDL)
13 第一塑料薄膜
14a、14b 金属丝网(金属多孔体)
15 第二塑料薄膜
16 粘接层
Claims (6)
1.一种固体高分子燃料电池用膜电极接合体,其特征在于是如下得到的,在于气体扩散层之间夹持两面具备催化剂层的高分子电解质膜并用第一塑料薄膜覆盖其外周缘部而成的层叠体的表面整面和背面整面配置金属多孔体,进一步用第二塑料薄膜覆盖所叠合的所述层叠体和金属多孔体的外周缘部,所述金属多孔体的外周缘部保持在第一塑料薄膜和第二塑料薄膜之间。
2.根据权利要求1所述的固体高分子燃料电池用膜电极接合体,其特征在于,在所述金属多孔体与第一塑料薄膜之间和/或在所述金属多孔体与第二塑料薄膜之间存在粘接层。
3.根据权利要求1或2所述的固体高分子燃料电池用膜电极接合体,其特征在于,在所述第一塑料薄膜与所述第二塑料薄膜之间存在粘接层。
4.根据权利要求1或2所述的固体高分子燃料电池用膜电极接合体,其特征在于,所述气体扩散层为微孔层。
5.根据权利要求3所述的固体高分子燃料电池用膜电极接合体,其特征在于,所述气体扩散层为微孔层。
6.一种固体高分子燃料电池,其特征在于,其具备权利要求1~5中任一项所述的膜电极接合体。
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PCT/JP2013/056780 WO2013137240A1 (ja) | 2012-03-14 | 2013-03-12 | 固体高分子形燃料電池用膜電極接合体 |
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JP6326862B2 (ja) * | 2014-02-26 | 2018-05-23 | 凸版印刷株式会社 | 膜電極接合体、燃料電池、及び膜電極接合体の製造方法 |
GB2530023A (en) * | 2014-09-02 | 2016-03-16 | Intelligent Energy Ltd | Fuel cell compression |
CN105304643A (zh) * | 2015-09-28 | 2016-02-03 | 深圳市华星光电技术有限公司 | 一种tft阵列基板及其制作方法 |
KR20180076661A (ko) * | 2016-12-28 | 2018-07-06 | 엘지디스플레이 주식회사 | 표시 장치용 기판과 그를 포함하는 표시 장치 |
DE102016226328A1 (de) * | 2016-12-29 | 2018-07-05 | Robert Bosch Gmbh | Gasverteilerplatte für eine Brennstoffzelle und Brennstoffzelle |
US10847826B2 (en) * | 2017-02-16 | 2020-11-24 | Panasonic Intelletual Property Management Co., Ltd. | Polymer electrolyte fuel cells and production method thereof |
DE202018104628U1 (de) * | 2018-08-10 | 2019-11-14 | Reinz-Dichtungs-Gmbh | Elektrochemisches System |
CN112448006B (zh) * | 2019-08-29 | 2023-02-03 | 未势能源科技有限公司 | 膜电极组件及其封装方法 |
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JP2005293944A (ja) * | 2004-03-31 | 2005-10-20 | Toyota Motor Corp | 燃料電池 |
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