CN1324502A - 制造气体扩散电极的丝网印刷方法 - Google Patents
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Abstract
本发明涉及一种制造气体扩散电极的丝网印刷方法,其中使用聚丁基丙烯-聚甲基丙烯-共聚物作为所述丝网印刷膏的结合剂。
Description
本发明涉及一种制造气体扩散电极的丝网印刷方法。
PEM燃料电池的核心部分是薄膜电极单元,它由一种两面具有电极的薄膜构成,所述电极包括一种电催化剂层。该电极优选具有一种固态的、透气并且导电的载体(碳纤维织物或者碳纤维纸),该载体优选采用一种聚合物悬浮体进行疏水化处理(该聚合物以下称为聚合物A,它涉及的聚合物例如是PTFE,即聚四氟乙烯、特氟纶)。在该载体上涂有一层电催化剂层,该层也具有疏水性。所以所述聚合物A不仅包含在载体中,也包含在所述电催化剂层中。
用于使电催化剂层具有疏水性的聚合物A的必要含量迄今为止通常是20-60%(重量百分比),其中较高含量的聚合物A,例如特氟纶会妨碍铂催化剂的活性,增高接触阻力,并且减小电极的空隙率(参见Watanabe的文章,《电分析化学杂志》,195(1985)81-83页),也就是说,它在***内起到不利的作用。所以用于使电催化剂层具有疏水性的聚合物A也被称为“催化剂阻碍剂”。
迄今为止,公知的电极除了有高含量的可使电催化剂层具有疏水性的聚合物A(20-60%重量百分比,始终相对于金属催化剂的含量)外,电催化剂层的厚度的均匀性也是一个问题。因此需要创造出一种合适的制造方法,它能以低成本和大批量方式制造出载体的均匀涂层,采用催化剂干粉,其层厚极小,为3-40微米。
按照公知的方法(参见Watanabe的文章,《电分析化学杂志》,195(1985)81-83页;《电分析化学杂志》,197(1986)195-208页;M.Uchida的文章,《电化学协会杂志》,142(1995)463-468页),将一种事先用聚四氟乙烯进行了疏水化处理的催化剂粉末制成的干粉混合物挤压到同样经过疏水化处理的载体上。为制造所述混合物,首先将碳粉与聚四氟乙烯分散体充分混合,然后在280℃以上的温度下干燥。其中除掉分散体中含有的表面活性浸润剂(Triton X 100)。使用该浸润剂的目的是补偿由于聚合物A在丝网印刷膏中的高含量而造成的变劣的加工特性。随后将混合物制成粉末。该方法十分繁琐,而且在技术上很难事先具有极小层厚的电催化剂层的均匀厚度,同时其生产量很小。该方法的缺点还在于:
-使电催化剂层具有疏水性的聚合物A的含量很高,并且
-处理中要加入浸润剂,随后要专门除掉,而且会留下有害的残余物。
丝网印刷是一种用于制造均匀薄层的公知技术。使用丝网印刷制造电化学***是公知的。根据美国专利文献US4229290,为此所使用的丝网印刷膏中含有特氟纶分散体,石墨和铂黑,为了稳定还添加了超过50%(重量百分比)的浸润剂或分散剂“Triton X 100”。用于疏水作用而添加到丝网印刷膏中的特氟纶成分约为25%(重量百分比),所以在得到的电催化剂层中也有这些数量。该丝网印刷膏被印刷在一种固体载体上、例如碳纸上,其中,也含有60%(重量百分比)的特氟纶。所以特氟纶的总含量约为85%。这种制造电极的方法的缺点是,除了使电催化剂层具有疏水性的聚合物A的含量过高外(这里是指特氟纶),还必须添加超过50%(相对催化剂膏的重量百分比)的浸润剂。
本发明的目的在于提供一种制造气体扩散电极的丝网印刷方法,其中所用的丝网印刷膏中不含浸润剂,并且或者不含聚合物A,或者聚合物A的含量很少(相对金属催化剂的重量百分比小于10%)。
本发明的目的通过独立权利要求所述的特征来实现。本发明的其他改进设计参见从属权利要求和说明书所述。
本发明的主题是一种制造气体扩散电极的丝网印刷方法,所采用的丝网印刷膏中含有的聚合物A的数量相对金属催化剂的重量百分比最大为10%,还包括至少一种金属催化剂和一种高沸点溶剂。
作为金属催化剂优选采用铂黑或碳基铂。
作为所述高沸点溶剂可采用一种酯和/或一种酮和/或一种醇,特别优选羟基醋酸丁酯,环己酮和/或萜品醇。
按照本发明的一个有利方案,所述丝网印刷膏中除了含有金属催化剂和高沸点溶剂外,还含有一种作为结合剂的聚合物B,优选是一种可加热到400℃的聚合物,特别优选的例如是聚丁基丙烯-聚甲基丙烯-共聚物。
按照一种方案,所述丝网印刷膏中含有少量的聚合物A,其重量百分比小于10%。
作为电催化剂层这里所指的优选是一层敷设在固态的、透气而且导电的电极载体上的电催化剂层,并且在其催化表面上产生燃料至质子的阳极氧化反应或者氧的阴极还原反应。所述电催化剂层包括至少一种金属催化剂,优选含有铂,它或者以铂黑的纯粹形式或者以铂在碳中的稀释形式加到催化剂膏中。所述电催化剂层中最好不要再包含其他成分,因为按照本发明的一个优选实施例,所述丝网印刷介质在处理时要加到催化剂膏内,然后通过干燥和加热从制成的,即成层的电极中除掉。
在进行处理时,所述丝网印刷膏(根据操作步骤也可称为碳膏或者催化剂膏)中至少还要含有一种高沸点溶剂作为丝网印刷介质,例如一种酯、酮和/或一种醇,特别是羟基醋酸丁酯,环己酮和/或萜品醇。作为丝网印刷介质的优选形式不要单独使用一种高沸点溶剂,而是添加一种聚合物B作为结合剂,例如添加聚丁基丙烯-聚甲基丙烯-共聚物,聚乙烯醇和/或聚乙烯氧化物。所述聚合物B最好是可加热的,特别是可加热到400℃的温度,或者仅残留不影响燃料电池工作的残余物。
所述电极是一种位于薄膜上的透气导电层,它优选是一种具有电催化剂层的载体。作为载体或衬底优选采用一种碳织物或者一种碳纸或者另外一种多孔的导电衬底。
通过称量出特定的铂含量,作为催化剂的纯铂黑为2-3mg/cm2,作为催化剂的碳基铂则根据碳中的铂含量为0.15-0.4mg/cm2。
在制造气体扩散电极时,完成了丝网印刷法以及随后的处理之后,用聚合物A(如特氟纶)对制成的电极进行疏水化处理。
然后用本发明所述气体扩散电极进行薄膜电极单元的电流电压曲线试验,所观察到的大电流强度下的电压降极小。其原因在于扩散阻力很小,这是由于聚合物A的含量少,而且多孔电催化剂层中的浸润剂残余物对疏水性的损害小。
所述丝网印刷法的特殊优点还在于改进了层厚的均匀性,因为所述催化剂膏中不含聚合物A时有更好的加工特性。
Claims (2)
1.一种制造气体扩散电极的丝网印刷方法,其特征在于,所采用的丝网印刷膏中包括至少一种金属催化剂和一种高沸点溶剂。
2.如权利要求1所述的方法,其特征在于,所述丝网印刷膏中含有作为聚合物B的聚丁基丙烯-聚甲基丙烯-共聚物。
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EP0641033B1 (de) * | 1993-08-31 | 1999-03-31 | Compur Monitors Sensor Technology GmbH | Verfahren zur Herstellung katalytisch wirksamer Gasdiffusionselektroden für elektrochemische Zellen |
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1999
- 1999-08-20 WO PCT/DE1999/002620 patent/WO2000013242A2/de active IP Right Grant
- 1999-08-20 CN CNB99812561XA patent/CN1195336C/zh not_active Expired - Fee Related
- 1999-08-20 ES ES99953554T patent/ES2214895T3/es not_active Expired - Lifetime
- 1999-08-20 DE DE59908263T patent/DE59908263D1/de not_active Expired - Lifetime
- 1999-08-20 EP EP99953554A patent/EP1118130B1/de not_active Expired - Lifetime
- 1999-08-20 CA CA2341494A patent/CA2341494C/en not_active Expired - Lifetime
- 1999-08-20 JP JP2000571099A patent/JP4707834B2/ja not_active Expired - Fee Related
- 1999-08-20 AT AT99953554T patent/ATE257621T1/de not_active IP Right Cessation
- 1999-08-20 CN CNB998125601A patent/CN1173426C/zh not_active Expired - Fee Related
- 1999-08-20 AT AT99953556T patent/ATE415713T1/de not_active IP Right Cessation
- 1999-08-20 JP JP2000571098A patent/JP4792160B2/ja not_active Expired - Fee Related
- 1999-08-20 WO PCT/DE1999/002622 patent/WO2000013243A2/de active Application Filing
- 1999-08-20 CA CA2341495A patent/CA2341495C/en not_active Expired - Lifetime
- 1999-08-20 DE DE59914914T patent/DE59914914D1/de not_active Expired - Lifetime
- 1999-08-20 ES ES99953556T patent/ES2315020T3/es not_active Expired - Lifetime
- 1999-08-20 EP EP99953556A patent/EP1118129B1/de not_active Expired - Lifetime
-
2001
- 2001-02-26 US US09/793,329 patent/US6645660B2/en not_active Expired - Lifetime
- 2001-02-26 US US09/793,411 patent/US20010018145A1/en not_active Abandoned
Cited By (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN104527247A (zh) * | 2014-01-03 | 2015-04-22 | 华东理工大学 | 基于丝网印刷技术的微流体燃料电池组微电路制备方法 |
CN104527247B (zh) * | 2014-01-03 | 2017-03-22 | 华东理工大学 | 基于丝网印刷技术的微流体燃料电池组微电路制备方法 |
Also Published As
Publication number | Publication date |
---|---|
WO2000013243A3 (de) | 2000-08-10 |
JP4792160B2 (ja) | 2011-10-12 |
WO2000013243A2 (de) | 2000-03-09 |
WO2000013242A2 (de) | 2000-03-09 |
DE59914914D1 (de) | 2009-01-08 |
CN1173426C (zh) | 2004-10-27 |
US20020022083A1 (en) | 2002-02-21 |
CA2341495C (en) | 2010-07-06 |
ES2315020T3 (es) | 2009-03-16 |
EP1118130A2 (de) | 2001-07-25 |
CA2341494A1 (en) | 2000-03-09 |
EP1118130B1 (de) | 2004-01-07 |
DE59908263D1 (de) | 2004-02-12 |
CA2341494C (en) | 2010-06-01 |
CN1195336C (zh) | 2005-03-30 |
ES2214895T3 (es) | 2004-09-16 |
US6645660B2 (en) | 2003-11-11 |
ATE257621T1 (de) | 2004-01-15 |
US20010018145A1 (en) | 2001-08-30 |
EP1118129B1 (de) | 2008-11-26 |
WO2000013242A3 (de) | 2000-06-08 |
JP2002525811A (ja) | 2002-08-13 |
EP1118129A2 (de) | 2001-07-25 |
ATE415713T1 (de) | 2008-12-15 |
JP2002525812A (ja) | 2002-08-13 |
CN1328707A (zh) | 2001-12-26 |
CA2341495A1 (en) | 2000-03-09 |
JP4707834B2 (ja) | 2011-06-22 |
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