CN1748334A - 具有隔膜分离器的燃料处理系统 - Google Patents

具有隔膜分离器的燃料处理系统 Download PDF

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CN1748334A
CN1748334A CNA2004800025323A CN200480002532A CN1748334A CN 1748334 A CN1748334 A CN 1748334A CN A2004800025323 A CNA2004800025323 A CN A2004800025323A CN 200480002532 A CN200480002532 A CN 200480002532A CN 1748334 A CN1748334 A CN 1748334A
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hydrogen
membrane separator
processing system
stream
fuel processing
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A·M·布伦纳
T·-C·于
Y·张
S·鲁夫
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Motors Liquidation Co
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Abstract

提供了一种用于对烃燃料进行重整的燃料处理系统。该燃料处理系统使用隔膜分离器以从重整产物流中分离出氢气。CO减少和清除系统与所述隔膜分离器一起作用以增加氢气的产生。

Description

具有隔膜分离器的燃料处理系统
技术领域
本发明涉及燃料处理系统，且更具体而言涉及具有用于帮助进行燃料重整的隔膜分离器的燃料处理系统。
背景技术
燃料电池已被提出用于多种应用，包括代替内燃机的电动车辆动力设备，的动力源。在质子交换膜(PEM)型燃料电池中，氢气被供应至燃料电池的阳极且氧气作为氧化剂被供应至燃料电池的阴极。质子交换膜燃料电池包括膜电极组件(MEA)，所述膜电极组件包括薄的可传送质子的非导电性固体聚合物膜-电解质，所述膜-电解质具有在其一个面上的阳极和在相对面上的阴极。膜电极组件被夹在一对导电元件之间，所述导电元件用作阳极和阴极的集电器，且包含在其中的用于将燃料电池的气体反应物分配在相应的阳极和阴极催化剂表面上的适当的通道和/或孔。在共同转让给Swathirajan等的美国专利Nos.5,272,017和5,316,817中对一种典型的质子交换膜燃料电池及其膜电极组件进行了描述。多个单个燃料电池通常被层叠在一起以形成质子交换膜燃料电池堆。
在质子交换膜燃料电池中，氢气(H2)被实施作为阳极反应物且氧气(O2)被实施作为阴极反应物。氧气可以纯氧的形式或作为空气(一种主要包括O2和N2的混合物)被供应。对于车辆应用，所希望的是使用液体燃料，例如甲醇、汽油、柴油等类似物，作为燃料电池的氢源。其它燃料包括乙醇和天然气。这些燃料优选用于车载储存且用以供应一些这种燃料的国内和国际基础设施中。然而，这些燃料必须进行分解用以释放其氢含量。分解反应通常在自动热重整器中完成。常规的典型工艺是蒸汽/汽油重整器，其中汽油和水(蒸汽)理想地进行反应以产生氢气和二氧化碳。也可能存在附加的组分例如一氧化碳。
燃料处理系统在本领域中是已公知的。通常的燃料处理系统通过使用一系列重整器以将烃燃料变成含氢重整产物流而发挥作用。这些重整器倾向于较大且难以进行封装。因此，所希望的是提供用于提取氢气的其它可选方式。
已公知的是可通过使用涂覆有钯或钯合金的隔膜从重整产物流中除去氢气。然而，氢分离隔膜倾向于不能提供燃料电池所需的用以保持与内燃机相匹敌的性能水平的氢气流。
因此，存在对具有减小的部件尺寸和不限制性能的氢分离装置的燃料处理系统的需求。
发明内容
本发明提供了一种与燃料处理系统一起使用的隔膜。所述燃料处理系统使用反应器以将烃燃料重整成含氢重整产物流。所述重整产物流流动通过隔膜分离器用以除去分解出的氢气。当前消耗了氢的剩余重整产物流动通过重整系统，所述重整系统进一步从重整产物流中分解出氢气。隔膜分离器允许减小重整系统的尺寸。从CO减少和清除系统上游的重整产物流中的氢气去除足以在这种下游系统中将更大量的重整产物转变成氢气。这种隔膜分离器和重整系统二者结合以将氢气分离出重整产物流的情况允许性能有所改进。
附图说明
从详细描述和附图中将更充分地理解本发明，其中：
图1是采用了根据本发明的第一实施例的隔膜分离器的燃料处理系统的示意图；
图2是根据本发明原理的隔膜分离器的透视示意图；
图3是根据本发明原理的隔膜分离器的透视示意图；
图4是采用了根据本发明原理的与水-气转换重整器结合成一体的隔膜分离器的另一种可选燃料处理系统的示意图；
图5是采用了根据本发明原理的与初级反应器结合成一体的隔膜分离器的第二种可选燃料处理系统的示意图；
图6是采用了根据本发明原理的隔膜分离器的燃料处理系统的细节示意图；和
图7是根据图6所示的燃料电池系统而使用的输水装置的示意图。
具体实施方式
下列对优选实施例的描述本质上仅是示例性的，且绝不是旨在限制本发明及其应用或使用。
本发明针对一种燃料电池系统10，包括燃料处理系统12和燃料电池堆14。现在将对燃料电池系统10进行描述，如图1-图6所示，其中共有的附图标记被用以表示相同或相似的元件。总的来说，燃料处理系统12包括自动热重整器16、隔膜分离器18、CO减少和清除部分20和燃烧器系统22。正如下面更详细地讨论的，燃料处理系统12作用以吸入燃料、空气和水，从而产生含氢气体。含氢气体随后用于燃料电池堆14中以便产生电流，正如本领域中已公知的。
现在参见图1，自动热重整器16包括初级反应器24。初级反应器24具有三个入口26、28和30。初级反应器24分别通过入口26、28和30接收燃料、空气和水。初级反应器24为任何能够对燃料进行化学重整，例如蒸汽重整、部分氧化或自动热重整，且能够输出重整产物中的氢气的类型。初级反应器24与隔膜分离器18流体连通用以将含氢重整产物流从自动热重整器16输运至隔膜分离器18。
隔膜分离器18与CO减少和清除部分20流体连通用以输运重整产物，且隔膜分离器18与燃料电池堆14流体连通用以传送纯氢或氢气-吹扫物混合物。
通常情况下，隔膜分离器18提供用于通过选择性地允许氢渗透通过隔膜而从气体混合物中除去氢气的机构。在授权给Edlund的美国专利No.6,152,995中对可用于该目的的典型的隔膜分离器进行了描述。隔膜分离器18受到所需组分在隔膜的进料侧和渗透侧之间的分压差的驱动。所需组分流是从高压进料侧到压力较低的渗透侧的。在存在钯或钯合金膜的情况下，氢选择性地可渗透通过致密的金属隔膜。可通过增加进料侧的氢分压、降低渗透侧的氢分压或减小金属隔膜的厚度而增加通过隔膜的氢的流量或流速。隔膜厚度上的限制由通过隔膜中的孔的可接受的漏泄率决定。这些孔减小了允许所有组分无选择性地通过的隔膜的选择性。隔膜分离器18中包含的膜材料是氢可渗透的材料例如钯或钯合金。合金包括，但不限于，钯-银或钯-铜。
可想到隔膜分离器18的任何构型是可使用的。两种用于隔膜分离器18和18′的可能构型为图2所示的管壳构型和图3所示的板状构型。
简要地参见图2，图中示出了隔膜分离器18的管壳构型，其中管状构型包括多条被封入壳体34中的管道32。管道32由钯、钯合金或支承材料上的钯层制成。所述支承材料可以是，但不限于，多微孔陶瓷、金属支承物或它们的组合。管道32上的钯或钯合金层的厚度小于10微米。钯或钯合金层还可被涂覆在支承管道的内部。来自自动热重整器16的重整产物通过管道32或在壳体34上通过而流动通过隔膜分离器18。所述流动可以是交叉流动、反向流动或同向流动。含钯管道32对于重整产物流中的非氢组分是不可渗透的。然而，氢气在钯中分解。渗透侧具有较低的氢分压且因此氢原子将自然地扩散通过隔膜且在低氢分压侧上重新结合，所述低氢分压侧为渗透侧。吹扫流可在隔膜的渗透侧上流动以从重整产物流中除去氢气。吹扫流通过具有比重整产物流更低的氢分压而实现该除去氢气的目的。氢气流受到进料侧和渗透侧之间的氢分压差的驱动。吹扫流可通过进一步降低渗透侧上的氢分压而增强渗透性能。因此，吹扫流将氢气从重整产物流中提取出来，留下与CO减少和清除部分20流体连通的贫氢重整产物流和与燃料电池堆14流体连通的富氢吹扫流。吹扫流可以是具有比重整产物流更低的氢分压的任何流。可通过改变管道直径、管道数量和管道长度而调节管状构型中的隔膜分离器18的表面积。增加管道32的表面积增加了可被提取的氢气量。此外，催化剂可被涂覆在壳体34上。
现在简要地参见图3，图中示出了隔膜分离器18′的板状构型。在该构型中，板36被层叠，在每层之间具有通道，且具有来自自动热重整器16的重整产物或在板36的相对侧上的富氢吹扫流。板36由钯、钯合金或支承材料上的钯或钯合金层制成。钯或钯层的厚度小于10微米。来自自动热重整器16的重整产物可以交叉流动、反向流动或同向流动的方式被供给进入板状构型隔膜分离器18′内。与隔膜分离器18中的含钯管道32相似的是，板36对于重整产物流中的非氢组分是不可渗透的。然而，氢气分解进入钯内。吹扫流具有较低的氢分压且因此当其在板36上流动时，氢原子扩散通过隔膜且在低氢分压侧上重新结合，所述低氢分压侧为渗透侧。因此，吹扫流将氢气从重整产物流中提取出来，留下与CO减少和清除部分20流体连通的贫氢重整产物流和与燃料电池堆14流体连通的富氢吹扫流。在板状构型中，可通过板的面积、板的数量以及通过歧管装置而调节隔膜分离器18′的表面积。增加板36的表面积增加了可由吹扫流提取的氢气量。此外，催化剂可被涂覆在板36或通道内的基层上。
参见图1，CO减少和清除部分20与隔膜分离器18流体连通且可包括水-气转换装置38和/或优先氧化反应器或PrOx 40或本领域中已公知的任何其它类型的CO减少和清除反应器中的至少一个。如图1所示，水-气转换装置38与隔膜分离器18流体连通，所述水-气转换装置的作用是从一氧化碳和水的反应中产生氢气。水-气转换38为一种平衡反应，所述平衡反应致使形成氢气。水-气转换装置38与优先氧化反应器(PrOx)40流体连通以输送含氢重整产物流。
优先氧化反应器40与水-气转换装置38流体连通，且被用以从由水-气转换装置38接收的重整产物中除去一氧化碳。优先氧化反应器40产生了堆级氢气。优先氧化反应器40与燃料电池堆14流体连通，且来自优先氧化反应器40的重整产物被传输至燃料电池堆14。
燃料电池堆14与CO减少和清除部分20和隔膜分离器18或18′流体连通。燃料电池堆14接收来自隔膜分离器18的富氢流且接收来自CO减少和清除部分20的贫氢重整产物。空气通过入口44进入燃料电池堆14。燃料电池堆14从氢气与来自空气的氧气的受控反应中产生电力和热量。燃料电池堆14与燃烧器系统22流体连通用以使空气与任何未使用的氢气、一氧化碳或烃发生反应。
参见图1，燃烧器系统22包括与燃料电池堆14流体连通的燃烧器46。具体而言，燃烧器46燃烧来自燃料电池堆14的剩余重整产物以产生用于自动热重整器16的热量。燃烧器46与自动热重整器16存在热传递关系，且将以来自燃烧器46的热气体形式存在的热量传送到自动热重整器16上，从而帮助保持自动热重整器16的初级反应器24的入口蒸汽温度。燃烧排出气体通过出口48排出燃烧器46。
在车辆操作中，燃料、水和空气进入初级反应器24且进行化学重整。来自初级反应器24的重整产物流入隔膜分离器18。隔膜分离器18从重整产物流中除去一些氢气。富氢渗透物从隔膜分离器18流入燃料电池堆14内。贫氢重整产物流流入水-气转换装置38内，且由重整产物流中的一氧化碳和水产生了更多的氢气。来自水-气转换装置38的重整产物进入优先氧化反应器40，其中一氧化碳进行选择性氧化。具有很少的一氧化碳的重整产物进入燃料电池堆14，其中所述重整产物与来自空气的氧气发生反应且进行化学反应，致使产生了电。未被燃料电池堆14使用的氢气重整产物流入燃烧器46内。燃烧器46使未使用的重整产物与空气混合并对其进行消耗，致使产生了用以使初级反应器24的蒸汽入口30变热的热量和通过出48排出系统的排出气体。
如图1所示，通过绕过水-气转换装置38和优先氧化反应器40而将堆级氢气直接送至燃料电池堆14，使得缩短了车辆运行的启动时间。进一步地，通过使用水-气转换装置38上游的隔膜分离器18，水-气转换反应的平衡可被进一步推向产物侧，导致产生更多的氢气，从而提高了效率。此外，通过隔膜分离器18除去氢气致使产生了更浓缩的反应物流且可减小水-气转换反应器38的尺寸或推动平衡以使得更少的一氧化碳被送至优先氧化反应器40，从而允许优先氧化反应器40更小。还可通过增加燃料处理器的工作压力，所述增加的工作压力对于隔膜分离器18而言是更好的操作点，而减小优先氧化反应器40和水-气转换反应器38的尺寸。
图4示出了燃料处理系统12的另一种可选实施例，所述燃料处理系统包括自动热重整器16、隔膜分离器18、CO减少和清除部分20和燃烧器系统22。然而，在该实施例中，隔膜分离器18被包含在水-气转换装置38内。在该第二实施例中，氢气在产生的同时被隔膜分离器18除去。该实施例提供了在单个单元中将水-气转换平衡更多地推向产物侧的优点。此外，该实施例致使更少的一氧化碳被送至优先氧化反应器40。
图5示出了本发明的燃料处理器的另一实施例，包括自动热重整器16、隔膜分离器18、CO减少和清除部分20和燃烧器系统22，然而，隔膜分离器18被设置在初级反应器24内。相似地，在该实施例中，氢气在产生的同时被隔膜分离器18除去。该实施例提供了推动蒸汽重整平衡以产生更多的氢气且致使减小水-气转换装置和优先氧化反应器的体积的优点。
图6示出了燃料电池系统100的另一个实施例，所述燃料电池系统被示意性地示出使用蒸汽作为吹扫气体。燃料电池系统100包括自动热重整部分102、隔膜系统104、CO减少和清除部分106、燃料电池堆系统108和燃烧器系统107。
自动热量整部分102包括自动热重整器110。自动热重整器110具有三个入口112、114和116，所述三个入口分别将燃料、空气和蒸汽带入自动热重整器110内。自动热重整器110通过导管111与隔膜系统104形成流体连通。隔膜系统104具有两个入口：一个是含氢重整产物111且另一个是蒸汽120。隔膜系统104具有三个出口：一个是空气/蒸汽流129，另一个是氢气流127，且再一个是重整产物流131。应该注意，流129可用以供应一些进料，所述进料换句话说由流114和116提供。
来自自动热重整系统102的含氢重整产物111进入如前面所论述的隔膜系统104中的隔膜分离器118。隔膜分离器118具有蒸汽入口120，所述蒸汽被用作吹扫气体以利于从混合重整产物流111中分离出氢气。来自入口120的蒸汽有利于从隔膜分离器118的表面中提取出氢气，由此产生包括蒸汽和氢气的流126。
氢气和蒸汽流126从隔膜分离器118被传送至隔膜系统104中的水蒸汽传输装置122。
参见图7，水蒸汽传输装置122具有多个在此示出作为三维通道的导管123。这些导管123被连接以便允许第一气体流通过所有导管123。第一流体的方向优选与第二气体流的方向相对。在该实施例中，第一气体流126包括蒸汽和氢气，且第二气体流128为空气，如图所示。装置122包括输水膜124，所述输水膜由允许将水蒸汽或蒸汽从一个流体流传输至另一个流体流的任何材料制成。这种材料选择性地允许传输蒸汽，而不同时允许传输其它气体例如氢气。通常情况下，输水膜124由包括那些由聚全氟磺酸、磺化聚苯乙烯、聚醚砜、磺化聚醚酮、聚碳酸酯、其它磺化材料及其混合物制成的材料制成。优选的膜材料包括聚全氟磺酸。特别优选的膜材料由E.I.Dupont deNemours公司出售，商标名称为“NAFION”。还在共有的申请，即于2001年7月20日申请的题目为用于燃料电池动力设备的水蒸汽传输装置的USSN 09/910,331和于2001年7月20日申请的题目为用于燃料电池重整器的水蒸汽传输装置的USSN 09/910,307中对水蒸汽传输装置进行了描述，以上每个所述申请在此作为教导工具被整体参考和引用。
输水膜124选择性地允许将蒸汽从包含氢气和蒸汽的流126传输至包含空气的流128，而不允许氢气从流126向空气流128的显著通过(泄漏)。具体而言，氢气和蒸汽流126进入水蒸汽传输装置122。空气流128也进入水蒸汽传输装置122。氢气和蒸汽的第一流126流动通过水蒸汽传输装置122的导管123并穿过隔膜124表面。第二空气流128流动穿过隔膜124的相对面。流126中的蒸汽被选择性地传输通过水蒸汽传输材料124并进入空气流128内以形成蒸汽和空气流129。通过从第一流126中除去蒸汽，氢气剩余在流127中。该氢气流127随后被送至燃料电池堆系统108。
隔膜分离器118的出口131与CO减少和清除系统106流体连通，用以传送贫氢重整产物流。CO减少和清除系统106可包括水-气转换装置130和/或优先氧化反应器132。水-气转换装置130与隔膜系统104流体连通，用以接收重整产物流。水-气转换130为平衡反应，所述平衡反应致使形成氢气。来自水-气转换装置130的重整产物流进入优先氧化反应器132。优先氧化反应器132被用以从在水-气转换装置130后接收的重整产物中除去一氧化碳。优先氧化反应器132与燃料电池堆系统108流体连通且产生了含有用于燃料电池堆系统108的氢气的堆级流135。
因此，燃料电池堆系统108与CO减少和清除系统106流体连通以接收包含氢气的堆级流135，且包括燃料电池堆134。除了从隔膜系统104供应的氢气流127之外，来自CO减少和清除系统106的氢气重整流135也进入燃料电池堆134内。燃料电池堆134具有空气入口136。燃料电池堆134从氢气和来自空气的氧气的受控反应中产生电力和热量。
本发明的描述本质上仅是示例性的，且因此未偏离本发明的要点的变型旨在处于本发明的范围内。这种变型不被视为偏离了本发明的精神和范围。

Claims (24)

1、一种燃料处理系统，包括：
用于将烃燃料流重整成包括氢和其它组分的重整产物流的反应器；
用于从所述重整产物流中除去氢气的隔膜分离器，所述隔膜分离器包括对于氢相对可渗透的且对于所述其它组分则渗透性相对较弱的隔膜；和
用于对所述重整产物流进行进一步重整的CO减少和清除系统。
2、根据权利要求1所述的燃料处理系统，其中所述CO减少和清除系统包括水-气转换装置和优先氧化反应器。
3、根据权利要求1所述的燃料处理系统，其中所述隔膜分离器包括多条用于使所述重整产物流动穿过所述隔膜以导致从所述重整产物流中分离出所述氢气的管道。
4、根据权利要求1所述的燃料处理系统，其中所述隔膜分离器包括用于有利于氢的选择性渗透的钯或钯合金。
5、根据权利要求4所述的燃料处理系统，其中所述钯或钯合金以限定出所述多条管道中的每条管道的表面的层的形式存在。
6、根据权利要求1所述的燃料处理系统，其中所述隔膜分离器包括多个用于使所述重整产物流动穿过所述隔膜以导致从所述重整产物流中分离出所述氢气的板。
7、根据权利要求6所述的燃料处理系统，其中所述钯或钯合金以限定出所述多个板中的每个板的表面的层的形式存在。
8、根据权利要求5或7所述的燃料处理系统，其中所述层小于10微米厚。
9、根据权利要求1所述的燃料处理系统，其中所述隔膜分离器与所述CO减少和清除系统结合成一体。
10、根据权利要求1所述的燃料处理系统，其中所述隔膜分离器与所述反应器结合成一体。
11、根据权利要求1所述的燃料处理系统，进一步包括吹扫流体系统，所述吹扫流体系统与所述隔膜分离器连通以利于从所述隔膜分离器输运氢气。
12、根据权利要求11所述的燃料处理系统，其中所述吹扫流体系统包括流，所述流具有比所述重整产物更低的氢分压用以引导从所述隔膜分离器中除去的氢气。
13、根据权利要求12所述的燃料处理系统，进一步包括输水装置，所述输水装置包括隔膜，所述隔膜对于水相对可渗透且对于所述氢则渗透性相对较弱用以从除去的氢气中分离出蒸汽。
14、根据权利要求13所述的燃料处理系统，其中所述输水装置进一步包括为引导从所述输水装置中分离出来的蒸汽而提供动力的空气源。
15、一种用于重整燃料的方法，包括以下步骤：
将烃燃料引入反应器内用以将所述烃燃料重整成包括氢和其它组分的重整产物流；
使所述重整产物流沿隔膜分离器通过用以从所述重整产物流中除去氢气；以及
将剩余的流引导至CO减少和清除系统用以进行进一步重整。
16、根据权利要求15所述的方法，进一步包括用流体对所述隔膜分离器的相对侧进行吹扫以从其中除去氢气的步骤。
17、根据权利要求15所述的方法，其中所述CO减少和清除系统包括水-气转换装置和优先氧化反应器。
18、根据权利要求17所述的方法，其中所述其它组分包括一氧化碳(CO)和水(H2O)且其中所述水-气转换装置使所述重整产物流中的所述CO和H2O进行反应，且所述优先氧化反应器从所述重整产物流中除去至少一部分的任何剩余一氧化碳。
19、一种燃料电池系统，包括：
用于将烃燃料流重整成含氢重整产物流的反应器；
用于从所述含氢重整产物流中除去氢气的隔膜分离器；
用于对所述重整产物流进行进一步重整的水-气转换装置；和
与所述隔膜分离器流体连通用以接收由所述隔膜分离器除去的氢气的燃料电池堆。
20、根据权利要求19所述的燃料电池系统，进一步包括在所述水-气转换装置下游的优先氧化反应器。
21、根据权利要求19所述的燃料处理系统，其中所述隔膜分离器与所述水-气转换装置结合成一体，由此提供了用于在所述转换反应器中形成所述氢气的同时除去所述氢气的钯基隔膜分离和水-气转换催化剂。
22、根据权利要求19所述的燃料处理系统，其中所述隔膜分离器与所述反应器结合成一体。
23、根据权利要求19所述的燃料处理系统，进一步包括吹扫流体，所述吹扫流体与所述隔膜分离器相连通以输运除去的氢气远离所述隔膜分离器。
24、根据权利要求12所述的燃料处理系统，其中所述流包括蒸汽。
CNA2004800025323A 2003-01-21 2004-01-20 具有隔膜分离器的燃料处理系统 Pending CN1748334A (zh)

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