CN110391432B - 燃料电池隔离件 - Google Patents
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Abstract
本发明提供导电性优异的燃料电池隔离件。所述燃料电池隔离件在基材上具有掺锑氧化锡膜，上述掺锑氧化锡膜含有15体积％且以上25体积％以下的聚(3,4－亚乙基二氧噻吩)/聚乙二醇(PEDOT/PEG)共聚物。
Description
技术领域
本发明涉及燃料电池隔离件。
背景技术
作为用于燃料电池的隔离件，已知通过压制加工等而形成的具有凹凸形状的隔离件。该隔离件被配置在成为单电池单元的膜电极接合体的气体扩散层上，气体扩散层侧的面构成形成反应气体等的流路的气体面，另一面构成形成冷却水等的流路的冷却面。该隔离件通常还具有导电性，以获取从单电池单元得到的电力。
另外，要求隔离件对膜电极接合体中产生的氢氟酸系酸等具有耐腐蚀性。
在日本特开2017－199535号公报中，作为导电性以及耐腐蚀性优异的燃料电池用隔离件，公开了一种具备具有凹凸形状的基板、以及形成在该基板的凹凸部的由导电性氧化物构成的CVD被膜的燃料电池用隔离件。在日本特开2017－199535号公报的实施例中，作为该CVD被膜，使用由氧化锡构成的被膜。另外，在日本特开2017－199535号公报的实施例中，对于导电性的评价，隔离件与作为气体扩散的碳片之间的导电性成为对象。
在日本特开平8－185870号公报中，作为具有良好的电导率且耐腐蚀性等优异的燃料电池用隔离件，公开了一种由以特定的金属陶瓷构成的基体和特定的金属氧化物的保护膜构成的固体电解质型燃料电池用隔离件，作为金属氧化物，例示出掺锑氧化锡。
在日本特开2017－112051号公报中，作为用于液晶、有机EL等的透明电极，公开了一种依次具有绝缘性基板、导电性金属氧化物的薄膜以及含有特定的聚噻吩的薄膜的透明电极。根据日本特开2017－112051号公报，为了改善表面平滑性，研究了在金属氧化物层上涂布含有特定的聚噻吩的薄膜。在日本特开2017－112051号公报中，作为该特定的聚噻吩，公开了通过聚苯乙烯磺酸等在噻吩中导入磺基而成的聚噻吩。
燃料电池为了获得所需的电压，以层叠上述单电池单元而成的堆叠方式使用。此时，各单电池单元所具备的隔离件彼此接触，要求该隔离件间的导电性。
为具有由导电性氧化物构成的被膜的隔离件的情况下，在与柔软的碳片之间，碳片因按压而柔软地变形而密合于隔离件，所以导电性容易变得良好。另一方面，隔离件即使按压也难以变形，所以难以改善隔离件间的导电性。
发明内容
本发明是鉴于这样的实际情况而完成的，提供导电性优异的燃料电池隔离件。
本实施方式所涉及的燃料电池隔离件在基材上具有掺锑氧化锡膜，上述掺锑氧化锡膜含有15体积％以上且25体积％以下的聚(3,4－亚乙基二氧噻吩)/聚乙二醇(PEDOT/PEG)共聚物。
本实施方式所涉及的燃料电池隔离件在基材上具有掺锑氧化锡膜，上述掺锑氧化锡膜含有聚(3,4－亚乙基二氧噻吩)/聚乙二醇(PEDOT/PEG)共聚物，上述掺锑氧化锡膜中的硫和碳的合计与锡的元素比[(S+C)/Sn]为0.6以上且1.1以下。
根据本发明，能够提供隔离件间的导电性特别优异的燃料电池隔离件。
根据下文给出的详细描述以及附图将更全面地理解本发明的上述和其他目的、特征和优点，其中详细描述和附图仅通过说明的方式给出，因此不应视为限制本发明。
附图说明
图1是表示本实施方式的燃料电池隔离件的一个例子的示意性截面图。
图2是表示本实施方式的燃料电池隔离件的使用状态的一个例子的示意性截面图。
图3是表示燃料电池隔离件的接触的一个例子的示意性截面图。
图4是表示构成隔离件的掺锑氧化锡膜中的(PEDOT/PEG)共聚物的含有比例与接触电阻和弹性模量的关系的图表。
图5是表示构成隔离件的掺锑氧化锡膜中的硫和碳的合计与锡的元素比[(S+C)/Sn]、与接触电阻的关系的图表。
具体实施方式
参照图1，对本实施方式的燃料电池隔离件的概要进行说明。图1的例子所示的燃料电池隔离件10在基材1上具有掺锑氧化锡(ATO)膜(2以及3)。
如图2的例子所示，本实施方式的燃料电池隔离件10被配置为气体面4侧与膜电极接合体20所具有的气体扩散层对置，形成气体流路，并且具有用于获取从膜电极接合体20得到的电力的导电性。
燃料电池为了获得所需的电压，通常以层叠上述膜电极接合体20而成的堆叠方式使用。如图3的例子所示，在堆叠膜电极接合体20的情况下，燃料电池隔离件10的冷却面5的至少一部分接触，构成接触部6。
本实施方式的燃料电池隔离件通过ATO膜含有15体积％以上且25体积％以下的聚(3,4－亚乙基二氧噻吩)/聚乙二醇(PEDOT/PEG)共聚物，从而减少掺锑氧化锡膜的弹力，提高隔离件的接触部6的导电性，并且提高基材1的耐腐蚀性。
以下，对本实施方式的燃料电池隔离件的各构成进行详细说明。
对构成隔离件的基材1的材质没有特别限定，能够从用作燃料电池隔离件的公知的材质中适当地选择而使用。作为一个例子，可举出塑料材料、金属基材等。从耐腐蚀性、导电性等方面来看，优选使用金属基材。对于金属基材的金属而言，作为一个例子，可举出铁、钛、铝、不锈钢等合金等，但并未特别限定。在耐腐蚀性的方面，优选钛或者不锈钢，从取得的容易性等来看，优选不锈钢。
基材的形状能够根据燃料电池的设计等而形成任意的形状。对于隔离件的形状，作为一个例子，可举出具有能够在膜电极接合体20侧形成气体流路的气体面4、能够在该气体面4的相反侧的面形成制冷剂等的流路的冷却面5的形状。
基材的厚度只要在确保气体的阻隔性、导电性的范围内适当地选择即可，例如能够设为0.05mm～0.2mm，优选0.1mm。
构成本实施方式的隔离件的ATO膜含有掺锑氧化锡和PEDOT/PEG共聚物，相对于整个膜，含有15体积％以上且25体积％以下的该PEDOT/PEG共聚物。
在ATO膜中，通过以上述特定比例含有具有导电性的PEDOT/PEG共聚物，从而能够对ATO膜赋予柔软性，提高隔离件间的接触部6的导电性。另外，由于PEDOT/PEG共聚物不具有磺基等那样的极性基团，所以能够抑制膜电极接合体20中产生的氢氟酸系酸、气体流路等中产生的盐酸系酸侵蚀基材，也能够提高隔离件的耐腐蚀性。
此外，如后述的实施例所示，在ATO膜中，相对于整个膜，含有15体积％以上且25体积％以下的PEDOT/PEG共聚物的情况下，该ATO膜中的硫和碳的合计与锡的元素比[(S+C)/Sn]为0.6以上且1.1以下。
ATO膜如图1所示可以形成在基材的两面，也可以仅形成在基材的气体面4侧，还可以仅形成在隔离件彼此接触的接触部6。从制造的容易性、导电性、基材的耐腐蚀性的方面来看，优选形成在基材的两面。
PEDOT/PEG共聚物优选是具有聚(3,4－亚乙基二氧噻吩)嵌段和聚乙二醇嵌段的嵌段共聚物。通过具有聚(3,4－亚乙基二氧噻吩)的嵌段而对共聚物赋予导电性。作为嵌段共聚物，可举出在聚(3,4－亚乙基二氧噻吩)嵌段的两端具有聚乙二醇嵌段的线性三嵌段、交替重复聚(3,4－亚乙基二氧噻吩)嵌段和聚乙二醇嵌段的线性多嵌段等。
PEDOT/PEG共聚物例如通过对3,4－亚乙基二氧噻吩进行聚合来形成聚(3,4－亚乙基二氧噻吩)的嵌段，接下来导入聚乙二醇，从而在末端形成聚乙二醇的嵌段的方法来合成，另外，也可以使用市售品。作为市售品，例如能够使用Aldrich制造的产品名AedotronC3－NM、产品名Aedotron C－NM等。
对掺锑氧化锡没有特别限定，例如能够适当地选择粒径1nm～500nm的粒子状的掺锑氧化锡来使用。
在本实施方式中，对在基材上形成ATO膜的方法没有特别限定，例如可以通过如下方式来形成：准备在溶剂中以所希望的比例配合掺锑氧化锡和PEDOT/PEG共聚物而成的涂布液，将该涂布液涂布于基材，并根据需要进行加热干燥来形成。
对涂布方法没有特别限定，例如可以从喷涂法、浸涂法、棒涂法、辊涂法、旋涂法等涂布方法中适当地选择。
对ATO膜的厚度没有特别限定，但从导电性以及耐腐蚀性的方面来看，优选为0.1左右。
实施例
以下，举出实施例、比较例详细地说明本实施，但本实施并不仅限于以下的实施例。
[实施例1]
作为基材，准备不锈钢(SUS447)板(厚度0.1mm)，作为掺锑氧化锡膜用的原料，准备掺锑氧化锡(粒径10nm，三菱材料制造，产品名T－1)和PEDOT/PEG共聚物硝基甲烷溶液(Aldrich制造，产品名Aedotron C3－NM)。
将上述基材设置于真空容器中，在真空条件下导入氩气，施加电压以使氩离子产生，轰击基材表面，从而除去表面的氧化被膜。
另外，准备在PEDOT/PEG共聚物硝基甲烷溶液中混合掺锑氧化锡粉末而成的混合溶液作为涂布液。掺锑氧化锡粉末的混合量调整为涂膜形成后的PEDOT/PEG共聚物的体积相对于整个膜成为15体积％。
接下来，在除去上述氧化被膜后的基材上通过旋涂法(1000rpm)涂布上述涂布液。接下来，加热到100℃，涂布硝基甲烷，从而形成具有ATO膜的基材。
[实施例2～3以及比较例1～3]
在上述实施例1的涂布液的调整中，通过变更掺锑氧化锡粉末的混合量，以使得PEDOT/PEG共聚物的体积相对于整个膜成为5、10、20、25以及30体积％的方式调整涂布液，除此以外，与实施例1同样地形成具有ATO膜的基材。
[比较例4]
在上述实施例1的涂布液的调整中，使用硝基甲烷溶剂来代替PEDOT/PEG共聚物硝基甲烷溶液，调整PEDOT/PEG共聚物的体积相对于整个膜为0体积％的涂布液，除此以外，与实施例1同样地形成具有ATO膜的基材。
＜接触电阻测定＞
准备两片实施例1的具有ATO膜的基材，使形成有ATO膜的面彼此重叠，每单位面积施加0.98MPa的压力并向基材间施加恒定电流，测定此时的电压值，并计算出电阻值。对于实施例2～3、比较例1～4，也同样地进行测定并计算出电阻值。将结果示于图4。
＜膜的弹性模量测定＞
对于实施例1～3以及比较例1～4的ATO膜，分别使用超微小硬度计(MTS Systems公司制造，Nano Indenter DCM)，通过纳米压痕法(连续刚性测量法)，测定压头的压入深度为10～15nm的弹性模量。压头使用金刚石制三棱锥压头。将结果示于图4。
＜膜的元素比的测定＞
对实施例1～3以及比较例1～4的ATO膜，分别通过X射线光电子能谱法(XPS)进行测定，并计算出元素比(S+C)/Sn。将该元素比与上述接触电阻的关系示于图5。
[结果的总结]
如图4所示，可观察到若ATO膜中的PEDOT/PEG共聚物的含有比例变高则膜的弹性模量降低的趋势。观察到若膜的弹性模量降低则接触电阻降低的趋势，但观察到若PEDOT/PEG共聚物的含有比例过高则接触电阻增大的趋势。推测这是因为由导电性高的氧化锡粒子构成的膜中的导电网络因PEDOT/PEG共聚物的比例变高而被破坏。如此，根据上述的实验结果，明确了通过掺锑氧化锡含有15体积％以上且25体积％以下的(PEDOT/PEG)共聚物，从而膜的弹性模量降低而隔离件间的密合性提高，并且氧化锡粒子的导电网络得到维持，获得隔离件间的导电性优异的本实施方式的隔离件。
另外，如图5所示，明确了在ATO膜中具有PEDOT/PEG共聚物的情况下，元素比(S+C)/Sn为0.6～1.1的范围在隔离件间的导电性优异的方面是优选的。
以上对本发明进行了详细描述，但显然本发明的各实施方式可以以许多方式进行改变。不应将这样的改变视为脱离本发明的精神和范围，并且对于本领域技术人员而言显然所有这样的修改都意图包括在本发明所要保护的范围内。
Claims (2)
1.一种燃料电池隔离件，在基材上具有掺锑氧化锡膜，
所述掺锑氧化锡膜含有15体积％以上且25体积％以下的聚(3,4－亚乙基二氧噻吩)/聚乙二醇即PEDOT/PEG共聚物。
2.一种燃料电池隔离件，在基材上具有掺锑氧化锡膜，
所述掺锑氧化锡膜含有聚(3,4－亚乙基二氧噻吩)/聚乙二醇即PEDOT/PEG共聚物，
所述掺锑氧化锡膜中的硫和碳的合计与锡的元素比[(S+C)/Sn]为0.6以上且1.1以下。
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