CN1313359C - 使用陶瓷技术的氢气发生器 - Google Patents

使用陶瓷技术的氢气发生器 Download PDF

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CN1313359C
CN1313359C CNB018148514A CN01814851A CN1313359C CN 1313359 C CN1313359 C CN 1313359C CN B018148514 A CNB018148514 A CN B018148514A CN 01814851 A CN01814851 A CN 01814851A CN 1313359 C CN1313359 C CN 1313359C
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fuel
zone
conversion zone
hydrogen generator
reformer
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CN1449360A (zh
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乔达里·R·克里珀拉
克里斯托弗·K·戴尔
斯蒂芬·P·罗杰斯
多米尼克·F·赫瓦西奥
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Motorola Mobility LLC
Google Technology Holdings LLC
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Motorola Inc
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    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
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Abstract

一种氢气发生器(10)，包括一限定了一个燃料重整器(14)的三维多层陶瓷载体结构(12)。该重整器包括一汽化区域(16)和一个含有催化剂的反应区域(18)。该重整器可作为蒸气重整器、部分氧化重整器或者自热重整器工作。该燃料重整器或处理器还包括一用于液体燃料的入口通道(20)和一用于富含氢的气体的出口通道(22)。燃料处理器是用多层陶瓷技术制成的，其中组装薄陶瓷层然后烧结而提供小型尺寸，其中封装的催化剂将输入的燃料重整或转化成富含氢的气体。

Description

使用陶瓷技术的氢气发生器
发明领域
本发明涉及氢气发生器，更特别地，涉及用多层陶瓷技术来提高尺寸和性能益处的氢气发生器。
发明背景
氢气是有吸引力的，并且已经在许多设备中用作燃料，如：在用于生产电力的燃料电池中，在包括火箭或内燃机的燃烧发动机中，及在包括用于精炼金属成分的化学处理设备中。一般来讲，氢气，或者更特别地，富含氢的气体，是用一般称作氢气发生器或重整器(reformer)的化学反应器从甲醇、天然气、石油或氨中加工的。重整的氢气燃料电池(RHFC)使用用燃料重整器从液体或气体碳氢化合物，如甲醇加工而成的富含氢的气体。
甲醇是用于燃料重整器或氢气发生器的优选燃料，因为相比于其它碳氢化合物燃料，如天然气、乙醇、石油、汽油或丁烷，甲醇更容易在相对较低的温度下重整成富含氢的气体，且产生的气态副产品(二氧化碳和一氧化碳)较少。这对于需要考虑重整器单元温度的小型便携式单元特别重要。将甲醇转化或重整成富含氢的气体通常是通过三种不同的重整过程中的一个来实现的。这三种是蒸气重整、部分氧化重整和自热重整。在这些类型中，蒸气重整对于甲醇重整是优选的，因为它最易于控制，产生的气态副产品(二氧化碳和一氧化碳)最少，且在较低的温度下产生较高的氢气产量，从而使自身有利于使用。在蒸气重整过程中，在存在水且应用热量的情况下，原始甲醇被催化转化成富含氢的气体。尽管蒸气重整是优选的工艺，但在许多情况下也使用部分氧化重整和自热重整。在部分氧化重整过程中，在有限量供应的氧气或空气以防止完全氧化的情况下，在催化剂上通过对甲醇进行部分氧化而将原甲醇转化成富含氢的气体。由于这是一个放热反应，它不需要输入热量来完成。如果甲醇和氧气与适当的催化剂接触，则不需要任何附加的热量输入就能够进行反应。对氧气局部压力和温度的控制非常重要，对于便携式甲醇重整，需要考虑重整器的更高的操作温度。
自热重整是催化部分氧化与蒸气重整过程的结合。在自热甲醇重整过程中，对产生热量的部分氧化反应进行仔细认真地控制，以提供充足的热量用于蒸气重整反应。在自热重整器中，在催化剂上方对输入的反应剂，即甲醇，与水和空气(或O2)之间的反应进行仔细认真地平衡，从而以最小量的CO生产出CO2和H2气体。在自热重整过程中，部分氧化步骤和蒸气重整步骤可在相同或不同的腔室中完成。
已经开发了燃料重整器与许多新型设备，包括燃料电池设备结合使用。这些燃料电池设备中的许多包括重整器，重整器一般是笨重和复杂的设备，包括若干由气体管路和硬件联接的分散部分，用于产生氢气。因此没有发现重整器适用于便携式电源应用，或者需要小尺寸和重量的其它应用。迄今为止，还没有开发出其中已经实现了重整器的小型化的利用陶瓷单块整体式结构的燃料重整器。现在已经普遍开发了使用低压层合陶瓷技术的包含小型通道和其它特征的层合陶瓷元件，用于微流体控制系统。由这些层合陶瓷元件制成的单块整体式结构提供了三维结构，这种三维结构对于化学反应成惰性且稳定，能够承受高温并提供小型结构，且电路或元件埋入或集成到这种陶瓷结构中的程度高，用于系统控制和功能性。此外，对于产生氢气而给小型燃料电池供料的微反应器设备中的催化剂支承，用于制成在结构中形成有微通道的陶瓷设备的陶瓷材料被认为是良好的候选者。
因此，本发明的一个目的是提供一种小型氢气发生器或燃料处理器，能够将燃料重整成富含氢的气体。
本发明的另一个目的是提供一种单块整体式结构，用于将燃料重整成富含氢的气体。
本发明的又一个目的是提供一种用陶瓷技术制成的单块整体式结构，从而实现多个内部管路互相联接和电路及联接件的集成。
本发明的再一个目的是提供一种氢气发生器或燃料处理器，它被小型化而与下列各项结合使用：(I)用于便携设备应用的燃料电池；(II)燃机；(III)化学处理设备；和(IV)其中富含氢的气体作为燃料消耗的其它设备。
发明概述
通过一种氢气发生器至少部分解决了上述和其它问题，并实现了上述和其它目的，该氢气发生器包括一限定了一个燃料重整器或燃料处理器的三维多层陶瓷载体结构。该燃料重整器包括一汽化区域和一个含有重整催化剂的反应区域。该燃料重整器是用多层陶瓷技术制成的，在该技术中组装薄陶瓷层然后烧结而提供小型尺寸，其中封装的催化剂将输入的燃料重整或转化成富含氢的气体。
本发明技术方案如下：
根据本发明，提供一种氢气发生器，包括：一个入口通道；一个汽化区域，该汽化区域接收来自入口通道的液体燃料；一个反应区域，该反应区域包括重整催化剂；至少一个蒸气通道，该蒸气通道用于将来自汽化区域中的蒸气输送到该反应区域；一个用于将富含氢的气体从该反应区域输出的出口通道；以及该入口通道、汽化区域、反应区域、至少一个蒸气通道和出口通道，所有这些一起构成一个燃料处理器内并一起形成在一个集成在一起的、烧结的、单块整体式陶瓷载体中。
优选地，还包括一集成在一起的热源，该集成在一起的热源使用传热通道与反应区域和汽化区域热耦接。
优选地，该集成在一起的热源包括一电驱动的电阻加热器。
优选地，该集成在一起的热源是一化学加热器，该化学加热器包括催化剂并设置成氧化燃料而产生热量。
优选地，该化学加热器还包括一空气入口，用于提供氧化燃料的氧气，入口通道包括一向化学加热器提供燃料的开口。
根据本发明，还提供一种氢气发生器，包括：一限定了一个燃料处理器的集成在一起的、烧结的、三维单块整体式多层陶瓷载体结构，该燃料处理器包括一汽化区域和一个包括重整催化剂的反应区域；该汽化区域和反应区域中的至少一个包括多个平行通道中的一个或者至少一个蛇形通道，该平行通道或蛇形通道形成在该集成在一起的、烧结的、单块整体式多层陶瓷载体结构中，以将液体燃料输送到汽化区域以及输送反应区域中的蒸气，该集成在一起的、烧结的、单块整体式陶瓷载体结构还包括一种电驱动的电阻加热器或一种包括催化剂并设置成氧化燃料而产生热量的化学加热器中的至少一个，该电阻加热器或化学加热器用导热通道与反应区域和汽化区域热耦接；一用于将该液体燃料引入燃料处理器中的入口通道；其中化学加热器接收来自入口通道的燃料并包括一个接收氧化燃料用的氧气的一个空气口；一用于将富含氢的气体从燃料处理器输出的出口通道；以及电阻加热器和化学加热器中的至少一个、汽化区域、反应区域、入口通道以及出口通道也形成在该集成在一起的、烧结的、单块整体式陶瓷载体中。
附图简介
权利要求中列出了相信是本发明的特征的新颖特征。但本发明自身及其其它特征和优点，将结合附图通过参照下面的详细说明而得到最佳理解，其中：
图1是根据本发明，包括多个通道的氢气发生器的简化正交视图；
图2是根据本发明的氢气发生器的一个替换实施例的简化正交视图；
图3是根据本发明的氢气发生器的一个替换实施例的简化正交视图；
图4是根据本发明的一个导热通道或通路的简化剖视图；
图5和6是根据本发明的热控制汽化器/反应区域通道的替换实施例的简化剖视图；
图7是根据本发明的重整燃料的方法的简化流程图。
优选实施例的描述
现在转向附图，特别是图1，以简化的正交图示出根据本发明的包括多个通道的氢气发生器10。氢气发生器10由一个三维多层陶瓷结构12构成。陶瓷结构12用多层层合陶瓷技术制成。结构12一般形成构成部件，这些构成部件而后以这样的方式烧结，从而提供一个单块整体式结构。陶瓷结构12中限定了一个大致用14表示的燃料重整炉或燃料处理器。燃料重整炉14包括一汽化室或汽化区域16，一反应室或反应区域18和一个合并集成的热源28。陶瓷结构12还包括至少一个与一组合溶液甲醇/水源24和一纯甲醇源26相联的燃料入口通道20，及一个富含氢气燃料出口通道22。应当理解，在不同实施例中，可使用分开的单独的甲醇和纯水燃料源。在这种情况下，可能需要甲醇与加热器直接相联，需要用一个混合器来混合甲醇和水燃料源。
在操作过程中，用导热通道或通路(目前讨论的)将热量从设备的中心区域，更特别地是从一集成加热器热源28有效地传递到反应区域18和燃料汽化器或汽化区域16。该特别实施例中，所描述的集成加热器28是一个化学加热器，包含催化剂，并设置成对燃料进行氧化而产生热量，但应当理解，电加热器的集成是本发明预想的。化学加热器28包括一空气口40，用于提供对燃料24和/或26进行氧化的氧气，和一个入口通道20，用于向加热器28提供燃料24和/或26。
来自燃料汽化器区域16的输出物经结构30运行到反应区域18，然后经过富含氢气气体的出口通道22。可选择地包括一个优先气体反应器21。在操作过程中，来自反应区域18的输出物运行到优先氧化反应器21，在此处从输出气体中将CO优先清除到低于30ppm用于燃料电池使用。可替换地，当使用高温燃料电池时，由于高温燃料电池可承受最大5％(摩尔(mol))的CO和甲醇的组合总量，结构10将不包括优先氧化反应器21。此外，结构10中还包括一废热回收区域34，用于通过一入口通道(未图示)从来自外部设备，如燃料电池组(未图示)，以及通过通道27从来自化学加热器28的用过的气体中收集热量。
一高效绝热器36环绕燃料重整器14定位，以保持外部温度较低用于包装，并将热量限定到燃料重整器。该特别实施例中，燃料处理器在从大气温度到300℃的温度范围内工作，除非它与高温燃料电池集成起来，在此情况下燃料处理器在140-300℃范围内工作。燃料汽化器区域16在120-160℃的温度范围内工作，反应区域18在200-250℃的温度范围内工作。此外，在燃料处理器10的该特别实施例中，包括一废气出口38，用于排出由设备10产生的废气。
应当理解，本发明也可以预想包括其它燃料输送装置和燃料汽化器、反应区域及化学加热器位置的替换实施例。特别预想的是这样一个实施例，其中预想只有一个单一燃料供应源，即甲醇和水源。单一甲醇和水溶液的使用能够制造出简单的结构，而不需要该设备装入两个燃料箱。尽管可以理解，特别是对于化学加热器来讲纯甲醇更有效且更优选，一摩尔水和1摩尔甲醇溶液也会工作，但严格意义上并不是认为操作有效。使用水和甲醇溶液的加热器适于实际应用，并可用一个简单的共用燃料箱来给加热器和重整器室供料。在这种情况下，燃料输送将被分成两个室，化学加热器28和燃料汽化器16。
下面，预想对于设备10的实际结构，特别是汽化器区域16、反应区域18和化学加热器28的实际位置的变化。在一个特别替换实施例中，预想反应区域18在两侧(顶侧和底侧)环绕化学加热器28。在另一个替换实施例中，预想可将反应区域18定位在加热器28下面，燃料汽化器区域16位于化学加热器28的顶部。此外，如前所述，预想化学加热器28还可以是电加热器(未图示)。
最后，本发明预想，尽管图1中所示的是这样一个结构，其中燃料电池没有与重整器14集成在一起，但可以附加地预想，燃料电池(未图示)可与氢气发生器10单块整体式集成在一起。在代理人记录号为CT00-014的与本申请同时提交并转让给同一受让人的名称为“利用陶瓷技术的集成有燃料电池的燃料处理器”的美国专利申请中，可以找到关于包括集成的燃料电池组的重整氢气燃料系统设备的其它信息，其被插入这里作为参考。
现在参照图2，示出大致以50表示的根据本发明的部分氧化氢气发生器。部分氧化重整器50对部分燃料进行氧化，向燃料重整器内的重整反应提供能量。直接传递热量使该重整器小而结构紧凑、重量轻且有动态响应。部分氧化系统依赖于以有限的氧气或空气供应量的原料反应，有限的氧气或空气供应目的是防止完全氧化。部分氧化是一个放热反应，在过程中，重整器的温度可超过400℃。对氢气部分压力的控制非常重要。部分氧化一般不用于甲醇重整器，更普遍的是结合温度可超过650℃的汽车应用的汽油重整器而利用。
如图所示，氢气发生器50包括通过入口54输入部分氧化反应器56的燃料52。操作过程中，首先用化学加热器或电燃烧器58在催化剂上对燃料52，一般是甲醇进行氧化。当部分氧化反应开始后，产生的热量将维持反应。不需要如参照图1所描述的蒸气重整器中那样提供附加的热量。操作过程中，需要对反应进行控制，从而不会进展到完全氧化。这是通过监测氧气局部压力和温度并通过控制空气入口60和燃料供给装置或入口54而实现的。
燃料52经过入口54运行到燃料重整器68，特别是第一部分氧化反应器56，然后经过通道62到达一第二部分氧化反应器64。富含氢气燃料出口66用于将已重整的氧气燃料引向一外部联接的燃料电池(未图示)。
一高效绝热器70环绕部分氧化反应器56和64定位，以保持外部温度较低用于包装，并保持将热量限定到燃料重整器。由本发明可以预想，虽然图2中所示的是燃料电池没有与重整器68集成的这样一个结构，但可以附加地预想，燃料电池(未图示)可与氢气发生器50单块整体式集成。该特别结构中，氢气发生器50包括一温度传感器72和一氧化局部压力，PO2传感器74。
如图2中所示，部分氧化氢气发生器50将氧气和甲醇大部分转化成带有少量一氧化碳的氢气和二氧化碳。由于部分氧化反应是一个放热反应，这个重整反应不需要增加热量。重整是在200℃-400℃温度范围内进行的。CO的清除是以与图1中所示蒸气重整器基本相同的方式完成的。
现在参照图3，所示的是一个大致以80表示的根据本发明的自热氢气发生器。自热重整是参照图1所述的需要热量输入的作为吸热反应的蒸气重整，与参照图2所述的产生热量的作为放热反应的部分氧化重整的结合。在自热重整中，实现了这两个重整过程的平衡。更特别地，自热重整将燃料82，更特别地是水、氧气和甲醇，转换成氢气和二氧化碳，而不需要增加热量。
燃料82经过入口81运行到燃料重整器83，更特别地运行到涉及对一些甲醇进行部分氧化的自热反应器87的第一阶段。燃料流经过通道88与涉及对甲醇进行蒸气重整的自热反应器90的第二阶段相互联接。这两个重整阶段可在同一腔室中发生，或者在两个相继的分离的腔室中发生。任何一种方式下，富含氢气的燃料出口92都用于将已重整的氧气燃料引向一外部联接的燃料电池(未图示)。
使用温度传感器84和氧气局部压力传感器85来监测反应过程。特别地，传感器84和85控制燃料供给(甲醇和水)82，及氧气供应源86。如果存在过多的氧气，则反应可向完全氧化推进，消耗过多的燃料，并产生不需要的过多的热量。相反，如果由于部分氧化反应而没有产生足够的热量，则炼焦会产生，阻碍蒸气重整过程。用适当的一种或一种以上的催化剂在200-300℃温度范围内完成自热甲醇重整。CO的清除是以与图1中所示蒸气重整器基本相同的方式完成的。
现在参照图4，所示的是用30表示的一传热结构的简化剖视图。如图所示，结构30由与一金属薄片104联接的通道102或通路构成，该金属薄片104与图1所示的区域18和28紧密接触。应当理解，这种类型的结构元件还用于在不同区域之间有效地传递热，其可能附加地包括在化学加热器28与燃料汽化区域16(如图1所示)之间以及在反应区域18与废热回收区域(34)(如图1所示)或者任何需要传热的其它区域之间传递热量。如图所示，导热结构30包括用于制造图1中用12表示的单块整体式结构的多层陶瓷层100。能够识别出化学加热器部分28和反应区域室18。导热厚片金属通路102高效地将顶部和底部部分热耦接，从而良好地传热。一与化学加热器区域28和反应区域18紧密接触的厚片金属层104扩展并对这些部分进行加热。
现在参照图5和6，在简化的截面图或平面图中示出燃料汽化器区域16的一部分。更特别地，图5中示出一蛇形通道110，该通道110一般由惰性多孔陶瓷材料填充或涂覆，用于热控制。可替换地，汽化器16可由多个与多孔扩散器113相联的带有用于热控制的惰性多孔陶瓷材料的平行通道112制成。在每种情况下，蛇形通道110或平行通道112在一端包括一个组合的单一液体入口进料装置114，在另一端116组合成一个单一蒸气出口。蛇形通道110和平行通道112形成在前面用12表示的多层陶瓷结构中。反应区域18包括如上所述在汽化器区域中发现的相似设计的通道和特征。更特别地，反应区域18包括一重整催化剂。该催化剂作为通道壁涂层或者作为催化剂颗粒的多孔致密层出现。一个设计目标是将反应通道的尺寸减小到气体扩散长度的范围，并控制有利于反应动力学的气体滞留时间或气体空间速度。大致类似于通道112的多个平行反应器通道提高了气体通过量，并减小了与通道阻塞相关的回压问题。应当理解，本发明可以预想，汽化器区域16和反应区域18可包括，任意数量的空腔或腔室，或者其通道、空腔或腔室的任意组合，来作为对蛇形通道110和平行通道112的附加，或者代替它们。
图7中以简化的流程图表示在蒸气重整氢气发生器，更特别地在图1中所示的设备10的重整器14中进行的化学反应120。如图所示，甲醇122和水124被输入大致与图1中的重整器14相似的蒸气重整器126中。蒸气重整器126在大约250℃的温度下工作，将输入的甲醇122和水124重整成一般称作富含氢的气体的重整气体混合物。更特别地，在存在催化剂，如氧化铜、氧化锌或氧化铜锌的情况下，甲醇122和水124溶液被重整成氢气、二氧化碳及一些一氧化碳。蒸气重整器126与可选择的一氧化碳清除器128配合操作，在存在优选的氧化催化剂和空气(或O2)的情况下，该一氧化碳清除将存在的一氧化碳的大部分重整成二氧化碳。已重整的气体混合物通过燃料输出口130将燃料供应到外部设备，如燃料电池。
因此，描述了一种包括一陶瓷载体的氢气发生器，该陶瓷载体限定了一个包括催化剂的反应区域。陶瓷载体还包括一与反应区域热耦接的热源。设置了一个入口通道，用于将液体燃料输入燃料处理器，和一输出通道，用于输出已重整的气体混合物。燃料处理器设备制成单块整体式集成结构，一般由多个薄陶瓷层构成，该多个薄陶瓷层组装然后以这样的方式烧结，以提供一个封闭的加热区域，其中封装的催化剂将输入的燃料重整成大多部分是氢的气体，这些氢气适于通过一适当的管路将燃料供应到与内部管路流体联通或者单块整体式集成在一起的其它外部设备。
尽管我们已经图示和描述了本发明的特定实施例，但本领域技术人员还是可以作进一步的修改和改进。因此我们期望能够理解，本发明并不限于所示的特定形式，我们期望附属权利要求覆盖不脱离本发明精神和范围的全部修改。

Claims (6)

1.一种氢气发生器，包括：
一个入口通道；
一个汽化区域，该汽化区域接收来自入口通道的液体燃料；
一个反应区域，该反应区域包括重整催化剂；
至少一个蒸气通道，该蒸气通道用于将来自汽化区域中的蒸气输送到该反应区域；
一个用于将富含氢的气体从该反应区域输出的出口通道；以及
该入口通道、汽化区域、反应区域、至少一个蒸气通道和出口通道，所有这些一起构成一个燃料处理器内并一起形成在一个集成在一起的、烧结的、单块整体式陶瓷载体中。
2.如权利要求1所述的氢气发生器，还包括一集成在一起的热源，该集成在一起的热源使用传热通道与反应区域和汽化区域热耦接。
3.如权利要求2所述的氢气发生器，其中该集成在一起的热源包括一电驱动的电阻加热器。
4.如权利要求2所述的氢气发生器，其中该集成在一起的热源是一化学加热器，该化学加热器包括催化剂并设置成氧化燃料而产生热量。
5.如权利要求4所述的氢气发生器，其中该化学加热器还包括一空气入口，用于提供氧化燃料的氧气，入口通道包括一向化学加热器提供燃料的开口。
6.一种氢气发生器，包括：
一限定了一个燃料处理器的集成在一起的、烧结的、三维单块整体式多层陶瓷载体结构，该燃料处理器包括一汽化区域和一个包括重整催化剂的反应区域；该汽化区域和反应区域中的至少一个包括多个平行通道中的一个或者至少一个蛇形通道，该平行通道或蛇形通道形成在该集成在一起的、烧结的、单块整体式多层陶瓷载体结构中，以将液体燃料输送到汽化区域以及输送反应区域中的蒸气，该集成在一起的、烧结的、单块整体式陶瓷载体结构还包括一种电驱动的电阻加热器或一种包括催化剂并设置成氧化燃料而产生热量的化学加热器中的至少一个，该电阻加热器或化学加热器用导热通道与反应区域和汽化区域热耦接；
一用于将该液体燃料引入燃料处理器中的入口通道；
其中化学加热器接收来自入口通道的燃料并包括一个接收氧化燃料用的氧气的一个空气口；
一用于将富含氢的气体从燃料处理器输出的出口通道；以及
电阻加热器和化学加热器中的至少一个、汽化区域、反应区域、入口通道以及出口通道也形成在该集成在一起的、烧结的、单块整体式陶瓷载体中。
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KR100823048B1 (ko) 2008-04-18
JP5000836B2 (ja) 2012-08-15
CN1449360A (zh) 2003-10-15
AU2001288522A1 (en) 2002-03-13
US7048897B1 (en) 2006-05-23
KR20030055255A (ko) 2003-07-02
WO2002018268A3 (en) 2002-06-06
TWI265142B (en) 2006-11-01
JP2004518598A (ja) 2004-06-24
WO2002018268A2 (en) 2002-03-07
EP1315669A2 (en) 2003-06-04

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