CN101682039B - 燃料电池和制造燃料电池的方法 - Google Patents
燃料电池和制造燃料电池的方法 Download PDFInfo
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Abstract
本发明涉及燃料电池,该燃料电池使用醇作为燃料,并包括电解质和位于电解质(10)两侧的阳极(20)和阴极(30)。该燃料电池的阳极含有催化醇降解的第一粒子(24,26)和催化醛降解的第二粒子(28)。
Description
技术领域
本发明涉及燃料电池。更具体地,本发明涉及使用醇作为燃料的燃料电池和制造这类燃料电池的方法。
背景技术
例如,日本专利申请公开2002-270209(JP-A-2002-270209)描述了具有阳极的聚合物电解质燃料电池,其阳极被构造成在使用非氢燃料时有优势。具体而言,在燃料电池的阳极表面上形成含生物化学催化剂的层。该生物化学催化剂层催化燃料原材料的降解而生成氢。
也就是说,如果例如使用甲醇作燃料,甲醇在经过该生物化学催化剂层时被降解。此时,在生物化学催化剂层中产生氢。在内侧(在电解质膜侧)向阳极供应氢以产生质子和电子。因此,根据上述相关技术,即使在使用醇(例如甲醇)作燃料时也供应纯氢,因此可以减轻由燃料中所含的碳化合物引起的阳极毒化。
如果燃料电池使用纯氢以外的燃料,例如醇,燃料中所含的氢比例低。因此,为了改进使用纯氢以外的燃料的燃料电池的发电性能,重要的是有效降解燃料和生成氢。为此,在JP-A-2002-270209、日本专利申请公开2004-71559(JP-A-2004-71559)和PCT申请2006-508519的公开日文译本(JP-A-2006-508519)中所述的相关技术中,通过在内侧向阳极供应在生物化学催化剂层中生成的纯氢来减轻阳极毒化。但是,在所述燃料电池中,未考虑生物化学催化剂层中生成氢的反应的效率和速率。为了通过改进燃料利用效率来改进燃料电池的发电性能,期望开发出可以以更高效率由燃料生成氢的电极。
发明概要
本发明提供了使用醇作为燃料的燃料电池,其发电性能通过提高燃料利用效率而获得改进。本发明还提供了制造这类燃料电池的方法。
本发明的第一方面涉及使用醇作为燃料的燃料电池。该燃料电池包括:电解质;位于电解质两侧的阳极和阴极对,且阳极含有催化醇降解的第一粒子和催化醛降解的第二粒子。
根据上述构造,即使该燃料电池使用醇作为燃料,所述第一粒子和第二粒子也会分两阶段降解醇,这提高了氢收率。因此,可以以更高效率利用燃料并改进燃料电池的发电性能。
在根据上述方面的燃料电池中,第一粒子可以含有醇脱氢酶。
通过采用醇脱氢酶,可以更可靠迅速地降解燃料,并提高燃料利用效率和燃料电池的发电性能。
在根据上述方面的燃料电池中,第一粒子可以含有Fe、Co、Ni、Fe-Co-Ni、Pt、Pt-Ru和Pt-Sn中的至少一种。特别地,第一粒子可以含有由Pt-RuPt-Ru构成的粒子。
通过采用这类粒子,可以由燃料可靠地生成氢。
在根据上述方面的燃料电池中,第二粒子可以含有乙醛脱氢酶。
这可以通过将醇降解过程中产生的醛进一步降解来生成氢。由此,可以提高燃料利用效率和改进燃料电池的发电性能。
在根据上述方面的燃料电池中,第一粒子和第二粒子都可以含有细胞色素P450。
在阳极处包含细胞色素P450可以有效降解醇和生成氢。细胞色素P450通过将醇直接降解成二氧化碳和水来提高氢生成效率。由此,可以提高燃料利用效率和改进燃料电池的发电性能。
在根据上述方面的燃料电池中,阳极可以包括载体,其中第一粒子和第二粒子负载在相同载体上。
这通过使第一粒子和第二粒子彼此靠近来提高醇降解反应和后面的醛降解反应的速率。由此,可以提高醇燃料利用效率和改进燃料电池的发电性能。
在根据上述方面的燃料电池中,第一粒子可以含有醇脱氢酶;第二粒子可以含有乙醛脱氢酶;且醇脱氢酶与乙醛脱氢酶的摩尔比值可以为0.25至4,更特别为0.25至1.5。
在根据上述方面的燃料电池中,电解质可以是阴离子交换膜。
本发明的第二方面涉及制造燃料电池的方法,该燃料电池使用醇作为燃料并具有阴离子交换膜作为电解质。该制造方法包括:将含有醇脱氢酶的第一溶液与含有乙醛脱氢酶的第二溶液混合;将通过混合第一溶液和第二溶液而获得的混合溶液干燥;将阴离子交换膜溶解在溶液中以形成电解质溶液;将通过干燥该混合溶液而获得的干燥物质与电解质溶液混合;和将与干燥物质混合的该电解质溶液施用到阴离子交换膜上。
在根据上述方面的制造燃料电池的方法中,该混合溶液中所含的醇脱氢酶与乙醛脱氢酶的摩尔比可以为0.25至4。
附图简述
从参照附图的下列示例性实施方案描述中,可以清楚看出本发明的前述和其它特征和优点,在附图中,使用类似数字代表类似元件,且其中:
图1是显示根据本发明一个实施方案的燃料电池的示意图;
图2是显示根据本发明实施方案的燃料电池的电极催化剂的图;
图3是显示制备根据本发明实施方案的燃料电池的电极催化剂的方法的流程图;
图4是显示根据本发明实施方案的燃料电池的I-V特性的图;
图5是显示电流密度随着根据本发明实施方案的燃料电池的催化剂中所含醇脱氢酶和乙醛脱氢酶的不同比例而变化的图表;且
图6是显示制备根据本发明实施方案的燃料电池的电极催化剂的另一方法的流程图。
实施方案详述
下面参照附图描述本发明的一个实施方案。在附图中,用相同或相应的标号表示相同或相应部件,以简化或省略其描述。
图1是显示根据本发明一个实施方案的燃料电池的构造的示意图。图1中所示的燃料电池是碱燃料电池。该燃料电池具有阴离子交换膜10(电解质)。阳极20和阴极30位于阴离子交换膜10的相对侧上。在阳极20和阴极30的外侧上都设有集电板40。与燃料供应源(未显示)相连的燃料通道50与阳极20侧上的集电板40相连。从燃料供应源经由燃料通道50和阳极侧的集电板40向阳极20供应燃料,未反应的燃料等由阳极20排放到燃料通道50。氧通道60与阴极侧的集电板40相连。经由氧通道60和阴极侧的集电板40向阴极30供应大气,含未反应的氧的大气废气由阴极30排放到氧通道60。
为了发电,向阳极20供应具有碳键并含氢的燃料,例如乙醇。在燃料供应到阳极20时,阳极20使燃料中的氢原子和已穿过阴离子交换膜10的氢氧根离子反应,这产生水并释放电子。阳极20处的反应在供应纯氢作为燃料时表示为下式(1),在供应乙醇作为燃料时表示为式(2)。
H2+2OH-→2H2O+2e-…·(1)
CH3CH2OH+12OH-→2CO2+9H2O+12e-…·(2)
向阴极30供应大气(或氧)。在大气供应到阴极30时,阴极30发挥其催化功能,使大气中的氧分子从电极接收电子以通过几个阶段生成氢氧根离子。氢氧根离子穿过阴离子交换膜10并移向阳极20侧。阴极30处的反应表示为式(3)。
1/2O2+H2O+2e-→2OH-…·(3)
总结上述在阳极20和阴极30处的反应,在燃料电池中总体发生下式(4)所示的生成水的反应。在该反应过程中,电子以电流形式流经阳极侧和阴极侧的集电板40,由此发电。
H2+1/2O2→H2O…·(4)
对碱燃料电池中所带的阴离子交换膜10没有具体限制,只要该介质允许由阴极30的电极催化剂生成的氢氧根离子(OH-)移向阳极20即可。阴离子交换膜10的具体实例包括具有阴离子交换基团(例如伯氨基至叔氨基、季铵基团、吡啶基、咪唑基、季吡啶鎓基和季咪唑鎓基)的固体聚合物膜(阴离子交换树脂)。合适的固体聚合物膜包括基于烃的树脂和基于氟的树脂。
对阴极30的构造没有具体限制,只要其催化由供给的大气生成氢氧根离子的反应即可。构成阴极30的催化剂的材料的实例包括:含有金属(例如铁(Fe)、铂(Pt)、钴(Co)和镍(Ni))的材料;一种或更多种这些材料负载在载体(例如碳)上的材料;具有这些金属的原子作为其中心金属的有机金属络合物;和其中这些有机金属络合物负载在载体上的材料。催化剂表面可以被由多孔材料等构成的扩散层覆盖。
阳极20被要求具有由所供应的燃料生成氢、并使氢与氢氧根离子反应生成水的催化功能。在使用醇作燃料时,重要的是由醇有效生成大量氢,以提高燃料电池的燃料利用效率。
已知的是,进入有机体的醇在从该有机体中排出之前通过酶的作用降解成二氧化碳和水。具体而言,醇,例如乙醇(CH3CH2OH),首先被醇脱氢酶(下文有时称作“ADH”)氧化成乙醛(CH3CHO)。在这种氧化反应过程中产生氢。
由乙醇生成的乙醛通过乙醛脱氢酶(下文有时称作“ALDH”)的活性进一步降解,生成乙酸。在生成乙酸时,产生氢。生成的乙酸然后进一步降解成二氧化碳和水。
如上所述,有机体具有催化使醇降解和生成氢的反应的酶。如果燃料电池使用醇燃料,可以采用这类酶作为催化剂,以有效降解醇燃料和生成氢。根据本发明实施方案的燃料电池的阳极20含有ADH和ALDH作为催化剂粒子。
图2是显示图1的虚线包围的区域II的放大视图的示意图。如图2中所示,阳极20由催化电极的载体(下文被称作“催化剂载体”)制成,其中数种类型的粒子负载在由碳等制成的载体22上。通过将催化剂载体与其中已溶有(或投入)与阴离子交换膜10相同的电解质膜的溶液混合、并将所得混合物施用到阴离子交换膜10的表面上来形成阳极20。
具体而言,载体22负载催化剂24和作为第一粒子的ADH 26和作为第二粒子的ALDH 28。催化剂24和ADH 26都催化乙醇降解生成乙醛和氢的反应。ALDH 28催化生成的乙醛降解生成氢的反应。
催化剂24、ADH 26和ALDH 28负载在相同载体22上。由于负载在相同载体22上,催化剂24、ADH 26和ALDH 28的各粒子可以在相同催化剂载体或在相邻催化剂载体上彼此邻近。因此,由于催化剂24和ADH 26的催化功能而由乙醇降解产生的乙醛可以立即被存在于催化剂24和ADH26附近的ALDH 28降解。由此,可以提高由乙醇生成氢的反应速率并迅速制成大量氢。
有机体具有多种类型的ADHs作为降解醇的酶。ADHs的具体实例包括ADH1、ADH2、ADH3、ADH4、ADH5、ADH6和ADH7。可以使用任何一种或多种这些ADHs作为第一粒子。
有机体也具有多种类型的ALDHs作为降解乙醛的酶。ALDHs的具体实例包括ALDH1A1、ALDH1A2、ALDH1A3、ALDH1B1、ALDH1L1、ALDH1L2、ALDH2、ALDH3A1、ALDH3A2、ALDH3B1、ALDH3B2、ALDH4A1、ALDH5A1、ALDH6A1、ALDH7A1、ALDH7A1P1、ALDH8A1、ALDH9A1、ALDH16A1和ALDH18A1。可以使用任何一种或多种这些ALDHs作为第二粒子。
图3是显示制备根据本发明实施方案的阳极的方法的流程图。在图3中,首先制备载体,其中催化剂24负载在载体22上(S102)。由于制备这类载体的方法是已知的,在此不作具体描述。然后,将步骤S102中制成的载体分散在分散液中以制备分散液A(S104)。
然后制备溶液A,在其中培养ADH 26(S110)。同样制备溶液B,在其中培养ALDH 28(S120)。由于培养这类酶的方法是已知的,在此不作具体描述。
然后,将含ADH 26的溶液A和含ALDH 28的溶液B混合,以制备混合溶液(S130)。确定溶液A与溶液B之间的混合比,以使所得混合溶液中所含的ADH 26与ALDH 28之间的摩尔比值为1∶4至4∶1,换言之,ADH 26摩尔数与ALDH 28的摩尔数的比率为0.25至4。然后,将该混合溶液与步骤S104中制成的分散液A混合,以制备分散液B(S132)。
将制成的分散液B搅拌(S134)。这使ADH 26和ALDH 28负载在载有催化剂24的载体22上。然后,将分散液B过滤,以提取其上载有各粒子的载体22。此后,将提取的载体干燥以制备催化剂(S138)。
此后,将催化剂与其中已溶有构成阴离子交换膜10的电解质膜的电解质溶液混合,并将所得混合物施用到阴离子交换膜10上。这样,就在阴离子交换膜10的表面上形成具有载体22的阳极20,载体22负载着催化剂24、作为催化剂的ADH 26和ALDH 28。为了避免热对ADH 26和ALDH28的破坏,上述方法中涉及ADH 26或ALDH 28的所有工艺(S110、S120、和S130至S138)都在70℃或更低、更优选60℃或更低的温度进行。
根据上述实施方案,使用由Pt-Ru或类似物制成的催化剂24、ADH 26和ALDH 28作为催化粒子。这通过有效破坏燃料中的乙醇中的C-C键来改进燃料效率。
图4是显示如上所述制成的燃料电池的I-V特性的图。在图4中,横轴代表电流密度[A/cm2],纵轴代表电压[V]。从图4中可以看出,根据该实施方案的燃料电池具有提高的发电性能,从而在整个电流密度范围内实现更高的电池电压。
图5是显示电流密度随着根据本发明实施方案负载在载体22上的ADH 26和ALDH 28量的不同比例而变化的图表。在图5中,使用ADH1作为ADH 26,并使用ALDH2作为ALDH 28。使用Pt-Ru作为催化剂24。催化剂24中所含的Pt与Ru之间的比例为Pt/Ru=58[重量%]。催化剂24中所含的Pt和Ru的体积比为Pt∶Ru=1∶2。
从图5中可以看出,在0.6[V]电压下,载体22上负载的ADH 26和ALDH 28之间的摩尔比值为40∶60的区域中,电流密度最高。ADH 26和ALDH 28之间的摩尔比不限于40∶60,并且可以不同于此。20∶80至80∶20的摩尔比,换言之,0.25至4的ADH 26与ALDH 28的摩尔数比率是特别有效的。20∶80至60∶20的摩尔比,换言之,0.25至1.5的ADH26与ALDH 28的摩尔数比率更优选。
制备根据本发明的催化粒子的方法不限于上述那种,且它们可以通过其它方法制备。图6是显示制备根据本发明实施方案的催化粒子的另一方法的流程图。
在图6的制备方法中,分散液A、溶液A和溶液B分别按照与图3所述相同的工艺中制备(S102至S104、S110和S120),此后通过将分散液A与溶液A混合来制备分散液C(S202)。此后,搅拌分散液C(S204)。这使催化剂24和ADH 26负载在分散液C中的载体22上。此外,在步骤S210中,通过将分散液C与溶液B混合来制备分散液D。此后,搅拌分散液D(S212)。这使得催化剂24、ADH 26和ALDH 28负载在分散液D中的载体22上。此后,进行与图3中的S136至S138相同的工艺以制备阳极20。
制备方法不限于图6的那种。例如,可以颠倒将溶液A混合和将溶液B混合的次序。也就是说,可以在步骤S202至S204中将分散液A与溶液B混合以制备分散液,并在搅拌所得分散液后,可以在步骤S210至S212中将其与溶液A混合以制备催化剂载体。
此外,在上述制备方法中,例如,分散液A的制备(S102至S104)、溶液A的制备(S110)和溶液B的制备(S120)可以以任何次序进行,只要这些分散液和溶液在其混合之前制成即可。
在上述实施方案中,将三种类型的催化粒子,即催化剂24、ADH 26和ALDH 28负载在单一载体上。但是,本发明不限于此。具体而言,由于催化剂24和ADH 26都具有主要降解醇的催化功能,可以使用催化剂24或ADH 26。也可以使用催化醇降解的其它催化剂或酶。例如,ADH 26可以被换成微粒体乙醇氧化酶(MEOS),其也已知为另一种降解醇的酶。
同样,也可以使用具有与ALDH 28相同或类似活性的其它酶、或催化乙醛降解的其它粒子。
此外,例如,可以使用直接将醇降解成二氧化碳和水的酶,例如细胞色素P450作为第一粒子和第二粒子。在这种情况下,催化剂24和细胞色素P450负载在载体22上,以使细胞色素P450将醇降解成乙醛并进一步降解乙醛以制氢。由此实现与如上所述相同的作用。
如果使用细胞色素P450,例如,可以如下所述制备催化剂。在图6的步骤S110中,作为溶液A,制备在其中培养细胞色素P450的溶液。省略步骤S120中的溶液B的制备。在后继步骤S202至S204中,将分散液A和溶液A混合和搅拌。此后,不进行步骤S210至S212,对搅拌过的混合物直接施以步骤S214至S216的工艺,以制备阳极20。
在上述描述中,使用Pt-Ru作为催化剂24。但是,根据本发明的催化剂24不限于此,可以含有例如Fe、Co、Ni、Fe-Co-Ni、Pt或Pt-Sn。
在上述实施方案中,阴极30的结构不同于阳极20。但是,本发明不限于此,且阴极30可以具有与阳极20相同的结构。电极20和30的表面可以被由多孔材料等构成的扩散层覆盖。
此外,在根据本发明实施方案中,燃料电池只有一个膜-电极组件(MEA),其中一对电极(阳极20和阴极30)位于阴离子交换膜10的相对侧上,且其中集电板40和反应气体通道50和60位于各电极的一侧上。但是,本发明的燃料电池不限于图1中所示的结构,并且可以具有堆叠结构,例如其中多个MEAs经由包括集电板的隔板串联。同样在这种情况下,通过为各MEA的阳极20提供如上所述载有催化剂24、ADH 26和ALDH28的催化剂载体,可以提高各MEA中的燃料利用并改进整个燃料电池的发电性能。此外,阳极20和阴极30的催化剂层的表面各自可以被扩散层覆盖。
在上述实施方案中,燃料电池是使用阴离子交换膜10的碱燃料电池。但是本发明不限于此,且燃料电池可以是使用可被负离子(例如KOH)渗透的电解质代替阴离子交换膜10的碱燃料电池。在这种情况下,可以通过降低电解质对过氧化氢离子的渗透性来降低电解质的劣化。尽管根据所述实施方案的电极有利地应用于碱燃料电池,但本发明不限于应用于碱燃料电池,并且可以应用于使用质子交换膜作为电解质膜的固体聚合物燃料电池,等等。同样在这种情况下,通过向阳极供应含醇并具有C-C键的燃料,可以改进燃料利用率。
在所述实施方案的上述描述中对各要素提到的数值、量、范围等仅是示例性的,且不应被视为限制性的。此外,该实施方案的上述描述中的结构、方法步骤等仅是示例性的,且不应被视为是本发明必不可少的。
Claims (8)
1.一种使用醇作为燃料的燃料电池,其特征在于包含:
电解质(10);和
位于电解质(10)两侧的阳极(20)和阴极(30),
其中:
阳极(20)含有催化醇降解的第一粒子(24,26)和催化醛降解的第二粒子(28);并且
第一粒子(24,26)含有Fe、Co、Ni、Fe-Co-Ni、Pt、Pt-Ru和Pt-Sn中的至少一种,
其中第一粒子(24,26)含有醇脱氢酶,其中第二粒子(28)含有乙醛脱氢酶,
其中阳极(20)包括载体,其中第一粒子(24,26)和第二粒子(28)负载在相同载体上。
2.根据权利要求1的燃料电池,其中第一粒子(24,26)含有Pt-Ru。
3.根据权利要求1的燃料电池,其中第一粒子(24,26)和第二粒子(28)均含有细胞色素P450。
4.根据权利要求1的燃料电池,其中醇脱氢酶与乙醛脱氢酶的摩尔比值为0.25至4。
5.根据权利要求4的燃料电池,其中醇脱氢酶与乙醛脱氢酶的摩尔比值为0.25至1.5。
6.根据权利要求1的燃料电池,其中所述电解质(10)是阴离子交换膜。
7.一种制造根据权利要求1至6任一项的燃料电池的方法,所述燃料电池使用醇作为燃料,并具有阴离子交换膜作为电解质(10),所述方法的特征在于包括:
将含有醇脱氢酶的第一溶液与含有乙醛脱氢酶的第二溶液混合;
将通过混合第一溶液和第二溶液而获得的混合溶液干燥;
将阴离子交换膜溶解在溶液中,以形成电解质(10)溶液;
将通过干燥所述混合溶液而获得的干燥物质与所述电解质(10)溶液混合;和
将与所述干燥物质混合的电解质(10)溶液施用到阴离子交换膜上。
8.根据权利要求7的方法,其中所述混合溶液中所含的醇脱氢酶与乙醛脱氢酶的摩尔比值为0.25至4。
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