CN105873854A - 使用钙钛矿作为其结构组分的重整器 - Google Patents

使用钙钛矿作为其结构组分的重整器 Download PDF

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Publication number
CN105873854A
CN105873854A CN201480072112.6A CN201480072112A CN105873854A CN 105873854 A CN105873854 A CN 105873854A CN 201480072112 A CN201480072112 A CN 201480072112A CN 105873854 A CN105873854 A CN 105873854A
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reformer
wall
cpox
perovskite
reforming reaction
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CN105873854B (zh
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C.M.芬纳蒂
P.德瓦尔德
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Watt Fuel Cell Corp
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Watt Fuel Cell Corp
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Abstract

重整器包括至少一个重整器反应器单元(300)，该重整器反应器单元(300)具有：拥有外表面(307)和内表面(306)的限制空间的壁，所述壁的至少一段以及由其限制的空间限定重整反应区(311)；用于将气态重整反应物的流接纳至所述重整反应区(311)的入口端(301)和相关的入口(302)；用于使在所述重整反应区中(311)制造的富含氢气的重整物流出的出口端(303)和相关的出口(304)，所述壁(305)的至少的与所述重整反应区对应的那段包括钙钛矿作为其结构组分，这样的壁段是透气性的以容许气态重整反应物在其中扩散和富含氢气的重整物从其扩散。

Description

使用钙钛矿作为其结构组分的重整器
相关申请的交叉引用
本发明申请要求各自在2013年11月6日提交的共同受让的共同未决的Finnerty等的美国临时专利申请序号61/900,510、61/900529、61/900543和61/900552的权益，将其全部内容引入本文作为参考。
技术领域
本教导涉及将可重整燃料重整以制造富含氢气的重整物的重整器和方法。
背景技术
可重整燃料向富含氢气的包含一氧化碳的气体混合物(通常被称为“合成气体”或“合成气”的产物)的转化可根据任意这样的公知燃料重整操作如蒸汽重整、干重整、自热重整、和催化部分氧化(CPOX)重整进行。这些燃料重整操作各自具有其与众不同的化学和要求并且各自以其相对于其它而言的优点和缺点为特点。
改进的燃料重整器、燃料重整器部件、和重整工艺的发展由于燃料电池(即，用于将可电化学氧化的燃料例如氢气、氢气与一氧化碳的混合物等电化学转化为电力的装置)的潜力而依旧是相当多的研究的焦点，对于包括主动力单元(MPU)和辅助动力单元(APU)在内的通常应用依旧起到大大扩展的作用。燃料电池也可用于专业化应用，例如，作为用于电动车的机载发电装置，用于住宅用装置的备用电源，用于在离网(out-of-grid)场所中的休闲用途、户外和其它耗电装置的主电源，和用于便携式电池组的更轻质、更高功率密度、不依赖环境温度的替代品。
由于氢气的大规模的经济的生产、其分销所需要的基础设施、以及用于其存储(尤其是作为运输燃料)的实用手段被普遍认为还有长的路要走，因此很多当前的研究和开发目的在于改进作为可电化学氧化的燃料(特别是氢气与一氧化碳的混合物)的来源的燃料重整器和作为这样的燃料到电力的转化器的燃料电池组件(通常被称为燃料电池“堆”)，以及重整器和燃料电池向用于产生电能的更紧凑、可靠和有效率的装置的集成。
发明内容
根据本发明，提供用于制造富含氢气的重整物的重整器，所述重整器包括至少一个重整器反应器单元，该重整器反应器单元具有：拥有外表面和内表面的限制空间的壁，所述壁的至少一段(section)以及由其限制的空间限定重整反应区(zone)；用于将气态重整反应物的流接纳至所述重整反应区的入口端和相关的入口；用于使在所述重整反应区中制造的富含氢气的重整物流出的出口端和相关的出口；所述壁的至少的与所述重整反应区对应的那段包括起到其结构组分作用的钙钛矿，这样的壁段是透气性的以容许气态重整反应物在其中扩散和富含氢气的重整物从其扩散。
采用若干种已知和常规的技术(例如，模塑、流延(铸造)、挤出、增材制造(additive manufacturing)、层合等)的任意者，钙钛矿与一种或多种其它材料一起或者在没有一种或多种其它材料的情况下可容易地形成为根据本教导的重整器的壁、或者壁的段。所得包含钙钛矿的壁结构可被制成为呈现出从良好到优异的机械和热性质，使得它们(所述性质)对于所有类型的重整器的壁/壁段的制作而言是特别有利的。
由于钙钛矿催化重整反应，特别是蒸汽重整、自热重整和部分氧化重整，因此它们作为用于形成催化重整器的壁或壁段的材料是尤其有用的。由于该本领，钙钛矿不仅提供催化重整器的机械和热稳定性性质或者对催化重整器的机械和热稳定性性质有显著贡献，它们还为重整反应供应催化剂(单独的或者与一种或多种其它重整催化剂组合)。与例如催化部分氧化重整器的放热的重整反应区对应的包含钙钛矿的壁结构能够非常好地忍受由发生在这样的区内的特征性地高的放热和由这样的重整器所常见的操作模式(启动、稳态和关停)中的快速和频繁的变化导致的机械和热应力。
由以下附图、描述、详述的示例性实施方式、和权利要求，将更充分地理解本教导的特征和优点。
附图说明
应理解以下描述的附图仅用于说明目的。附图未必是按比例的，重点通常放在说明本教导的原理上。附图绝不意图限制本教导的范围。相似的附图标记通常是指相似的部分。
图1和2为根据本发明的重整器(分别为具有多个催化部分氧化重整器反应器单元的液体燃料催化部分氧化重整器和气态燃料催化部分氧化重整器)的图示。
图3A和3B分别为重整器反应器单元(比如，图1和2的催化部分氧化重整器中的那些)的放大的纵截面图和横截面图。
图3C和3D为根据本教导的重整器反应器单元的两其它实施方式的放大的横截面图。
图4为图1中所示的重整器的歧管和相关的(关联的，associated)重整器反应器单元的部分的放大的纵截面图。
图5为包括根据本教导的包含钙钛矿的重整器的总体上圆柱形的管式固体氧化物燃料电池的等距视图(isometric view)。
具体实施方式
将理解，本文中的本教导不限于所描述的具体程序、材料、和改动并且因此可变化。还将理解，所使用的术语仅用于描述具体实施方式的目的并且不意图限制本教导的范围，本教导的范围将仅由所附权利要求限制。
在整个本申请中，当组成(组合物)被描述为具有、包括或包含特定部件(组分)时，或者当方法被描述为具有、包括或包含特定方法步骤时，所思虑到的是，这样的组成(组合物)还基本上由所列举的部件(组分)构成或者由所列举的部件(组分)构成，和这样的方法还基本上由所列举的方法步骤构成或者由所列举的方法步骤构成。
在本申请中，当一个要素(元件)或部件(组分)被认为包括在所列举的要素(元件)或部件(组分)的列表中和/或选自所列举的要素(元件)或部件(组分)的列表时，应理解，所述要素(元件)或部件(组分)可为所列举的要素(元件)或部件(组分)的任一个，或者所述要素(元件)或部件(组分)可选自所列举的要素(元件)或部件(组分)的两个或更多个。进一步地，应理解，在不背离本教导的焦点和范围的情况下，本文中所描述的组成(组合物)、设备、或方法的要素(元件)和/或特征可以多种方式组合，无论是在其中言明的还是未言明的。例如，当介绍具体的结构(体)时，该结构(体)可在本教导的设备和/或方法的多种实施方式中使用。
术语“包括”、“包含”、“具有”、“含有”、或“含”(包括其语法等同物)的使用应通常被理解为是开放式的和非限制性的，例如，不排除另外的未列举的要素(元件)或步骤，除非另有具体叙述或者由上下文理解。
本文中单数例如“一个(种)(a，an)”和“该(所述)”的使用包括复数(并且反过来也成立)，除非另有具体叙述。
当在数量值之前使用术语“约”时，本教导也包括所述具体数量值本身，除非另有具体叙述。如本文中使用的，术语“约”指的是与标称值的±10％变化，除非另有指示或暗示。
应理解，步骤的顺序或者用于进行某些动作的顺序是不重要的，只要本教导仍然是可操作的。例如，此处描述的方法可以任何合适的顺序进行，除非本文中另有指示或者明显与上下文矛盾。此外，可同时进行两个或更多个步骤或者动作。
在本说明书中的多个位置处，值是以集合或者以范围公开的。具体意图是，本文中公开的数值的范围包括在所述范围内的每一个值以及其任意子范围。例如，在0-20范围内的数值具体地意图单独地公开0、1、2、3、4、5、6、7、8、9、10、11、12、13、14、15、16、17、18、19、和20，以及其任意子范围，例如0-10、8-16、16-20等。
本文中提供的任意和全部实例、或示例性语言例如“比如(例如)”的使用仅意图更好地阐明本教导且不对本发明的范围加以限制，除非有声明。本说明书中的语言均不应被理解为将任何未声明的要素指示为对于本教导的实践是必要的。
指示空间方位或高度的术语和表述例如“上部”、“下部”、“顶部”、“底部”、“水平(的)”、“竖直(的)”等除非它们的上下文用法另有指示，否则在本文中应被理解为不具有结构、功能或操作意义并且仅反映附图的某些中所说明的本教导的液体燃料CPOX重整器的多种视图的任意选择的方位。
术语“陶瓷”除了其本领域公认的含义之外在本文中还应被理解为包括玻璃、玻璃-陶瓷、和金属陶瓷(即，陶瓷-金属复合物)。
表述“透气性的”在其在本文中应用于CPOX反应器单元的壁时应被理解为意味着能透过气态CPOX反应混合物和气态产物重整物(包括如下而没有限制：气态CPOX反应混合物的气化的液体或者气态可重整燃料组分和产物重整物的氢气组分)的壁结构。
表述“液体可重整燃料”应被理解为包括在经历重整时进行向富含氢气的重整物的转化的在标准温度和压力(STP)条件下为液体的可重整的包含碳和氢的燃料，例如，甲醇、乙醇、石脑油、馏出物、汽油、煤油、喷气发动机燃料、柴油、生物柴油等。表述“液体可重整燃料”应进一步理解为包括这样的燃料，无论它们处于液态还是气态即蒸气。
表述“气态可重整燃料”应被理解为包括在经历重整时进行向富含氢气的重整物的转化的在STP条件下为气体的可重整的包含碳和氢的燃料，例如，甲烷、乙烷、丙烷、丁烷、异丁烷、乙烯、丙烯、丁烯、异丁烯、二甲基醚、它们的混合物例如天然气和液化天然气(LNG)(其主要为甲烷)、以及石油气和液化石油气(LPG)(其主要为丙烷或丁烷，但是包括主要由丙烷和丁烷组成的所有混合物)等。
术语“重整器”应被理解为包括其中发生一种或多种导致可重整燃料转化为富含氢气的重整物的重整反应的任何装置或设备。术语“重整器”因此适用于其中发生如蒸汽重整、干重整、自热重整、催化部分氧化(CPOX)重整这样的操作或者两种或更多种这样的重整操作的组合的反应器并且适用于具有内部重整能力的燃料电池。
表述“重整反应”应被理解为包括在可重整燃料向富含氢气的重整物的重整或转化期间发生的反应(一种或多种)。
表述“重整反应混合物”指的是包括如下的混合物：气化的液体可重整燃料、气态可重整燃料或者其组合；氧化剂，例如，作为空气供应的氧气，和在蒸汽或自热重整的情况下，蒸汽。
表述“催化重整”应被理解为指的是在重整催化剂存在下进行或者可在重整催化剂存在下进行的任意和全部重整反应并且具体地包括如下而没有限制：蒸汽重整、自热重整和催化部分氧化(CPOX)重整。
图1和2说明针对CPOX重整的根据本教导构造的重整器的实施方式。这些重整器实施方式仅用于说明目的并且不应被认为限制本发明的范围。
如图1中所示，液体燃料CPOX重整器100包括用于将包含氧气的气体(在此处以及在本教导的其它实施方式中通过空气来示例)引入到导管103中并且用于驱动这个和其它气态物流(包括气化的液体燃料-空气混合物和富含氢气的重整物)通过所述重整器的多种气流通道的离心式鼓风机102。导管103可包括流量计104和热电偶105。这些和类似装置可安置在液体燃料气相CPOX重整器内的多种位置处以监测和控制其操作。
在示例性的液体燃料气相CPOX重整器100的操作的启动模式中，通过离心式鼓风机102引入到导管103中的处于环境温度的空气穿过第一加热区106，在第一加热区106中在给定的流速下，所述空气初始地被(例如电阻型的)第一加热器107加热至在预设的、或者目标的升高温度的第一范围内。所述经初始加热的空气然后穿过热传递区108，热传递区108在CPOX重整器100的操作的稳态模式中被从发生在管式CPOX反应器单元109的气相CPOX反应区110内的气相CPOX反应回收的放热热所加热。一旦实现了重整器100的这样的稳态操作，即，在CPOX反应器单元109内的CPOX反应变成自持时，可减少第一加热器107的热输出或者停止其操作，因为进来的空气已经通过穿过热传递区108而被加热至在其升高温度的第一范围内、或者接近其升高温度的第一范围。
在导管103内继续进一步地下游，已经通过在操作的启动模式期间穿过第一加热区106或者通过在操作的稳态模式期间穿过热传递区108而经初始加热的空气穿过第二加热区111，在第二加热区111中其进一步被第二加热器112(其也可为电阻型)加热至在升高温度的第二范围内。第二加热器112可操作以完成(top-off)先前被加热的空气的温度，从而满足液体燃料CPOX重整器100的若干操作要求，即，在快速响应和按需的基础上辅助所述重整器的热需求的调节和微调，提供足够的热用于在进一步地下游被引入到导管103中的液体可重整燃料的随后气化和提供经加热的气态CPOX反应混合物。
将液体可重整燃料比如柴油经由泵113通过装备有任选的流量计115和任选的流量控制阀116的燃料管线114连续地引入并且进入到导管103中，在导管103中所述燃料通过利用来自从第二加热区111流出的经加热的空气的热的气化器系统117而被气化。经气化的即现在气态的燃料与经加热的空气的物流在导管103的混合区118中组合。在导管103的混合区118内设置混合器例如静态混合器比如在线混合器119、和/或形成于导管103的内表面内的涡流产生用螺旋形凹槽、或者以外部方式供以动力的混合器(未示出)以提供与否则的情况相比更均匀的燃料-空气气态CPOX反应混合物。
经加热的气化的燃料-空气混合物(经加热的气态CPOX反应混合物)进入歧管或送气室(增压室，plenum)120，其起到将所述反应混合物更均一地和例如以更均匀的温度分布到管式气相CPOX反应器单元109(结合图4A-4D中所示的CPOX反应器单元的代表性实施方式更详细地描述其包括包含钙钛矿的CPOX催化剂的壁结构)中的作用。导管103和歧管120通常被热绝缘体包围以防止通过这些结构的热损失。
从歧管120，将经加热的CPOX反应混合物引入到管式气相CPOX反应器单元109中。在CPOX重整器100的操作的启动模式中，点火器123引发包含钙钛矿的管式CPOX反应器单元109的CPOX反应区110内的气态CPOX反应混合物的CPOX反应，从而开始富含氢气的重整物的制造。一旦已经实现稳态CPOX反应温度(例如，250℃-1,100℃)，反应变成自持的并且可停止所述点火器的操作。提供热电偶124和125以分别监测发生在导管103内的气化操作和发生在CPOX反应器单元109内的气相CPOX反应的温度，温度测量结果作为所监测的参数被转发(分程传递，relay)给重整器控制系统126。
重整器100还可包括电流来源例如可再充电的锂离子电池系统127，以为其电驱动部件比如鼓风机系统102，流量计104和115，加热器107和112，液体燃料泵113，流量控制阀116，点火器123，以及热电偶105、122、124和125提供动力，并且如果需要，存储电力用于后续使用。
如果需要，可将来自液体燃料CPOX重整器100的产物流出物或富含氢气的重整物引入到一个或多个常规的或者以其它方式知晓的一氧化碳除去装置128中以减少其一氧化碳(CO)含量，例如，当要将所述产物流出物作为燃料引入至使用特别易被CO中毒的催化剂的燃料电池堆例如聚合物电解质膜燃料电池时。因此，例如，可将所述产物流出物引入到水煤气变换(WGS)转化器中，在其中CO被转化为二氧化碳(CO2)，并且同时产生额外的氢气，或者可将所述产物流出物引入到其中使CO经历向CO2的优先氧化(PROX)的反应器中。也可采用这些工艺的组合(例如，WGS之后为PROX，以及反过来)进行CO减少。
如下也在本教导的范围内：通过使所述产物重整物穿过装备有提供将所述产物重整物分离为氢气物流和包含CO的副产物物流的氢气选择性膜的已知的或常规的清除单元或装置而降低所述产物重整物中的CO的水平。该种类的单元/装置也可与一种或多种其它CO减少用单元例如前述WGS转化器和/或PROX反应器组合。
如图2中所示，气态燃料CPOX重整器200包括用于将空气引入到导管203中并且用于驱动这个和其它气态物流(包括气态燃料-空气混合物和富含氢气的重整物)通过所述气相CPOX重整器的多种通道(包括开放的气流通道)的离心式鼓风机202。导管203可包括流量计204和热电偶205。这些和类似装置可安置在CPOX重整器200内的多种位置处以监测和控制其操作。
在示例性的气态燃料CPOX重整器200的操作的启动模式中，通过离心式鼓风机系统202引入到导管203中的空气与从气态燃料存储罐213通过装备有任选的热电偶215、流量计216和流量控制阀217的燃料管线214以相对低的压力引入到导管203中的气态可重整燃料比如丙烷组合。空气和丙烷在导管203的混合区218中组合。在导管203的混合区218内设置混合器例如静态混合器比如在线混合器219、和/或形成于导管203的内表面内的涡流产生用螺旋形凹槽、或者以外部方式供以动力的混合器(未示出)以提供与否则的情况相比更均匀的丙烷-空气气态CPOX反应混合物。
所述丙烷-空气混合物(即，气态CPOX反应混合物)进入歧管或送气室220，其起到将所述反应混合物更均一地分布到包含钙钛矿的管式CPOX反应器单元209(其相应的实施方式详细地示于图3A-3D中)中的作用。在CPOX重整器200的操作的启动模式中，点火器223引发管式CPOX反应器单元209的CPOX反应区210内的气态CPOX反应混合物的气相CPOX反应，从而开始富含氢气的重整物的制造。一旦已经实现了稳态CPOX反应温度(例如，250℃-1,100℃)，反应变成自持的并且可停止点火器的操作。接近于一个或多个CPOX反应区210布置热电偶225以监测发生在CPOX反应器单元209内的CPOX反应的温度，温度测量结果作为所监测的参数被转发给重整器控制系统226。
重整器200还可包括电流来源例如可再充电的锂离子电池系统227，以为其电驱动部件比如离心式鼓风机系统202、流量计204和216、流量控制阀217、和点火器223提供动力。
如在CPOX重整器100的一氧化碳除去装置128的情况中那样，气态燃料CPOX重整器200可包括可类似地操作的一氧化碳除去装置228。
图3A和3B分别说明适合于引入到重整器(比如图1和2的CPOX重整器)中的根据本教导的管状CPOX反应器单元300的放大的纵截面图和横截面图。
如图3A和3B中所示，催化重整器比如液体或气态燃料CPOX重整器的重整器反应器单元300包括用于接纳气态CPOX反应混合物的流的入口端301和相关的入口302、用于流出富含氢气的重整物的出口端303和相关的出口304、和包括一种或多种钙钛矿(单独地或者与一种或多种另外的组分比如难熔的金属、催化惰性的陶瓷、耐高温粘合剂和不同于钙钛矿的重整催化剂一起)作为其结构组分的透气性壁305。包含钙钛矿的透气性壁305进一步包括内表面306、外表面307以及由壁305、更具体地由内壁表面306限制的开放的气流通道308。
开放的气流通道308通过容许基本上不受阻碍的、气态反应混合物的流入和包含氢气的重整物的流出而有助于在所述重整器内维持低的背压。因此，在根据本教导的重整器的操作中，不超过约3英寸水(0.0075巴)、例如不超过约2英寸水、或者不超过约1英寸水的背压是可容易实现的。
如果需要的话，并且在所显示的反应器单元300的实施方式中，所述反应器可划分成两个主要区域(region)：从入口端301延伸至重整反应区311并且基本上没有重整催化剂的第一或上游区域309和对应的壁段310；以及与放热的重整反应区311有共同边界的第二或下游区域312，并且仅其对应的壁段313包括钙钛矿(与另外的材料一起或者无另外的材料)作为其结构组分。第二区域312可从其与第一区域309的边界延伸至出口304或者出口304附近。相对于反应器单元300的整个长度，第一和第二区域309和312的长度可显著变化。因此，例如，第一区域309可延伸达反应器单元300的长度的约20％-约60％例如约30％-约50％，并且第二区域312延伸达所述CPOX反应器单元的长度的剩余部分。
将反应器单元300划分为第一和第二区域容许热的重整反应在很大程度上被限制于第二区域312和将第一区域309保持在(例如，在从环境到最高达约350℃的区域中的)明显较低的温度下，特别是在反应器单元300的燃料-空气混合物入口端301与图1的液体燃料CPOX重整器100的歧管120以及图2的气态燃料CPOX重整器200的歧管220的接合点处。基本上没有催化剂的第一区域309的该较低的温度(该温度低于许多热塑性树脂的熔融温度并且低于许多热固性树脂的热降解温度)使得使用若干家族的热塑性和热固性树脂的任意者来制造歧管成为实际的和有利的。可用于制作前述歧管120和220的热塑性和热固性树脂的具体类型包括聚醚酰亚胺(PEI)、聚芳基醚酮(PAEK)比如聚醚醚酮(PEEK)、酚醛树脂等。这些和其它热稳定树脂除了它们相对低的材料成本之外还具有如下的附加优点：能采用低成本制造程序例如挤出模塑、真空模塑、注射模塑、反应注射模塑、旋转模塑等容易地成型为复杂形状，并且因此很好地适合于制造具有相对复杂的几何结构的歧管。
为了防止或抑制产物氢气通过透气性壁305而损失，可将氢气阻挡物314附着至所述壁的整个外表面307，或者至少的与重整反应区311对应的壁段313的外表面。能够充当有效的氢气阻挡物的材料应当是在重整反应所典型的温度下热稳定的并且应当足够致密以防止或者阻止重整物气体特别是氢气渗透或者扩散通过其。满足这些要求的多种陶瓷材料(包括玻璃和玻璃-陶瓷)和金属是已知的并且因此适合于提供氢气阻挡物314。用于氢气阻挡物314的具体材料包括，例如，铝、镍、钼、锡、铬、氧化铝、重结晶氧化铝、铝化物、铝硅酸盐、二氧化钛、碳化钛、氮化钛、氮化硼、氧化镁、氧化铬、磷酸锆、二氧化铈、氧化锆、莫来石等、其混合物以及其层状组合。
当构成氢气阻挡物314的材料的性质允许时，所述氢气阻挡物可作为预先形成的层、箔、薄膜或膜施加至反应器单元壁的外表面的至少的与重整反应区对应的那部分。所述氢气阻挡物可用耐高温粘结剂粘合至所述壁。替代地，可通过采用任何合适的沉积方法，例如，常规或者以其它方式知晓的陶瓷-涂覆和金属-涂覆技术(比如喷涂、粉末涂覆、刷涂、浸渍、流延、共挤出、金属化等)的任意者，以及它们的许多变型的任意者在外表面上形成氢气阻挡物314。氢气阻挡物的厚度的合适范围将主要取决于所选择的阻挡物材料的氢气渗透性(透气性)特性以及围封所述重整反应区的壁的透气性特性，这样的厚度是本领域技术人员采用已知的和常规的实验技术容易确定的。对于许多阻挡物材料和包含钙钛矿的反应器壁结构，氢气阻挡物314的厚度可从约2微米到约15微米，例如，在约5微米到12微米之间变化。
如本领域技术人员将容易认识和领会的，重整反应器单元的截面构型和尺度，以及在具有多个这样的反应器单元或者这样的反应器单元的阵列的重整器中反应器单元的数量和从它们的几何中心或者质心测量的它们彼此隔开的距离将取决于具体的重整反应器的操作和机械性能规格而产生。在基本上均匀的环形截面的重整反应器单元(例如图3A和3B中所示的重整器反应器单元300)的情况下，所述透气性壁的长度、内径和外径(限定透气性壁的厚度)以及附着至所述透气性壁的外表面的氢气阻挡物的位置、长度和厚度将由尤其是如下决定：所述重整器的氢气产生本领，其本身又是包括如下的若干因素的函数：类型、量(可存在于所述透气性壁内的重整催化剂即钙钛矿和任何其它重整催化剂的负载量和分布)、所述壁的多孔结构的特性(影响所述壁的透气性并且因此影响重整反应的特性)比如孔体积(孔径的函数)、孔的主要类型(主要是开放的即网状的还是主要是封闭的即非网状的)、和孔形状(球形的还是不规则的)、重整反应混合物的体积流速、重整反应温度、背压等。
此外，氢气阻挡物可为与CPOX反应器单元的透气性壁(例如，至少的包含CPOX催化剂的壁段)的外表面关联的加压流体比如加压气体。在足够压力的情况下，在CPOX反应器单元外部的加压流体可产生防止氢气通过形成CPOX反应器单元的透气性壁而损失的阻挡物。加压流体典型地为加压气体比如惰性气体(例如，氮气)和/或空气。使用加压空气作为氢气阻挡物具有如下的附加的优点：氧气从CPOX反应器单元的外部扩散至内部，该扩散的氧气可调节将要和/或正被重整的气态CPOX反应混合物的O:C比，特别是当在CPOX反应区周围使用和存在这样的氢气阻挡物时。
在某些实施方式中，所述CPOX反应器单元除了其入口和出口之外都可位于气密室中，从而允许在CPOX反应器单元外部的环境中的流体比如气体的加压，该加压气体可产生与CPOX反应器单元的外表面关联的氢气阻挡物。在具体实施方式中，由于直到CPOX反应区才在CPOX反应器单元中产生氢气，因此仅有所述CPOX反应器单元的CPOX反应区被围封在被流体比如空气加压的气密室中。在其中CPOX反应区未延伸至CPOX反应器单元的出口的实施方式中，可将CPOX反应区的开头部分到出口围封在气密室中以允许使用加压气体作为氢气阻挡物。在一些设计中，如本文中描述的室可围绕CPOX反应区的一部分，同时可存在围绕CPOX反应区的剩余部分的另一形式的氢气阻挡物。
在其中使用室比如气密室的实施方式中，可使用与所述室的内部流体连通的导管以用流体对所述室进行加压。例如，加压流体或气体导管可提供所述(气密)室的内部与加压或压缩流体的来源(比如压缩气体例如压缩空气的容器)之间的可操作的流体连通。
重整器反应器单元300除了图3B中所示的环形截面之外还可采取其它截面构型比如示于图3C和3D中的那些。图3C说明具有交替的凹面-凸面或双叶(二裂片，bilobate)截面的重整器反应器单元。具有这样的截面构型的重整器反应器单元可为尤其有利的，其中它们的出口段将如在Finnerty等的共同未决的、共同受让的、公布的美国专利申请No.2013/0230787(其全部内容引入本文作为参考)的燃料电池组件中那样与类似地配置的管式固体氧化物燃料电池单元接合或者配对。
具体重整器的期望的机械性能特性将在相当大程度上取决于如如下的这样的因素：用于构造所述重整器反应器单元的钙钛矿和如果使用的其它材料的热和机械性质、所述重整器反应器单元的壁的透气性结构的孔的体积和形态、所述重整器反应器单元的尺度特别是壁厚、和如本领域技术人员将认识和领会的相关因素。
为了使重整器合适地运行，所述至少一个重整器反应器单元的包含钙钛矿的催化活性的壁结构的透气性性质必须为这样的：其容许可重整燃料自由地进入和扩散通过这样的壁结构，从而不仅与表面催化剂，而且也与内部催化剂进行有效接触。应注意，对于可重整燃料具有有限的透气性的重整器反应器单元壁结构可为传质受限的，从而显著地阻碍所述燃料向富含氢气的重整物的重整。相形之下，合适透气性的包含钙钛矿的催化活性的反应器壁结构促进可重整燃料的重整以及对于期望组成的富含氢气的重整物的制造的选择性。通过本教导来指引和采用已知的和常规的试验程序，本领域技术人员可容易地构造具有对于所要处理的具体的可重整燃料呈现出最优的透气性性质的包含钙钛矿的壁结构的重整器。
钙钛矿对于重整反应比如蒸汽重整、自热重整和CPOX重整具有催化活性并且因此不仅对于催化重整器的与它们的重整反应区对应的壁结构的制作是有用的，它们还可供应重整催化剂的部分或者甚至全部。
在本文中可使用任意的常规的和以其它方式知晓的钙钛矿来构造所有类型的重整器的壁和/或壁段，包括催化和非催化种类的那些。合适的钙钛矿描述于例如如下中：美国专利No.4,321,250、4,511,673、5,149,516、5,447,705、5,714,091、6,143,203、6,379,586、7,070752、7,151,067、7,410,717、和8,486,301，和公布的美国专利申请2012/0161078、2012/0189536、和2012/0264597，将其全部内容引入本文作为参考。
钙钛矿催化剂是在本教导中有用的一类重整催化剂，因为它们还适合于构造催化重整器的催化活性的壁结构。钙钛矿催化剂特征在于结构ABX3，其中“A”和“B”为具有非常不同尺寸的阳离子，且“X”为与两种阳离子都键合的阴离子(通常为氧)。合适的钙钛矿CPOX催化剂的实例包括LaNiO3、LaCoO3、LaCrO3、LaFeO3和LaMnO3。
钙钛矿的A部位改性通常影响它们的热稳定性，而B部位改性通常影响它们的催化活性。钙钛矿可针对具体的催化重整反应条件通过在它们的A和/或B部位处掺杂而定制改性(tailor-modified)。掺杂导致活性掺杂剂在钙钛矿晶格内的原子水平分散，从而抑制它们的催化性能的退化。钙钛矿还可呈现出在作为催化重整的特征的高温下对硫的优异的容忍性。作为重整催化剂有用的掺杂的钙钛矿的实例包括La1-xCexFeO3、LaCr1-yRuyO3、La1-xSrxAl1-yRuyO3和La1-xSrxFeO3，其中取决于掺杂剂的溶解度极限和成本，x和y为范围例如0.01-0.5、0.05-0.2等的数。可用于构造本文中的重整器的壁/壁段的一些具体钙钛矿为锰酸锶镧(LSM)、铁酸锶镧(LSF)、铁酸钴锶镧(LSCF)、锰酸钙镧(LCM)、铬酸锶镧(LSC)、镓锰酸锶镧(LSGM)、它们与彼此的以及与其它钙钛矿的混合物。
在重整器壁/壁段的制作中采用的钙钛矿的总量可在相当宽的界限内变化，条件是这样的量对它们的机械强度有显著贡献。通常，所述重整器的整个壁，或者在其重整反应区限于第二区域312的CPOX重整器反应器300的情况下，仅有与CPOX反应区311对应的壁段313，可包含至少20重量％例如至少50重量％，和在其它实施方式中，至少80重量％且最高达100重量％钙钛矿。
本教导还思虑任选地另外使用任意的迄今为止常规的和以其它方式知晓的非钙钛矿CPOX催化剂和催化剂体系。在本文中可任选地使用的许多已知的和常规的非钙钛矿重整催化剂之中有公开于例如如下中的金属、金属合金、金属氧化物、混合金属氧化物、烧绿石、它们的混合物以及组合(包括其多个种类)：美国专利No.5,149,156；5,447,705；6,379,586；6,402,989；6,458,334；6,488,907；6,702,960；6,726,853；6,878,667；7,070,752；7,090,826；7,328,691；7,585,810；7,888,278；8,062,800；和8,241,600，将其全部内容引入本文作为参考。
虽然许多高度活性的包含贵金属的重整催化剂是已知的并且因此在本文中可为有用的，但是由于如下，它们通常与其它已知类型的重整催化剂相比不太常用：它们高的成本、它们在高温下烧结并且因此经历催化活性降低的趋向、以及它们被硫中毒的倾向。
除了钙钛矿和其它任选的重整催化剂之外，根据本教导构造的重整器的壁和壁段也可由其制作的其它材料包括常规的和以其它方式知晓的难熔的金属、陶瓷、耐高温粘合剂以及其组合。
所述有用的金属中有钛、钒、铬、锆、钼、铑、钨、镍、铁等、它们与彼此的和/或与其它金属和/或金属合金等的组合。
陶瓷由于如下而对于重整器壁结构的构造而言是尤其有吸引力的一类材料：与对于该目的也是有用的许多难熔的金属和金属合金相比，它们相对低的成本。这样的陶瓷可比较容易采用已知的和常规的孔形成程序形成为完全可再现的孔类型的管式透气性的结构、以及陶瓷的通常高度令人满意的结构/机械性质(包括热膨胀系数和热冲击性能)、以及耐化学退化性使得它们是特别有利的材料。合适的陶瓷包括CPOX反应器单元的整个壁结构)包括，例如，尖晶石，氧化镁，二氧化铈，稳定化的二氧化铈，二氧化硅，二氧化钛，氧化锆，稳定化的氧化锆例如氧化铝-稳定化的氧化锆、氧化钙-稳定化的氧化锆、二氧化铈-稳定化的氧化锆、氧化镁-稳定化的氧化锆、氧化镧-稳定化的氧化锆和氧化钇-稳定化的氧化锆，氧化锆稳定化的氧化铝，烧绿石，钙铁石，磷酸锆，碳化硅，钇铝石榴石，氧化铝，α-氧化铝，γ-氧化铝，β-氧化铝，硅酸铝，堇青石，铝酸镁等，其多种公开于美国专利No.6,402,989和7,070,752(其全部内容引入本文作为参考)中；以及，稀土铝酸盐和稀土镓酸盐，其多种公开于美国专利No.7,001,867和7,888,278(其全部内容引入本文作为参考)中。
对于重整器的壁/壁段的制作可为有用的耐高温粘合剂包括常规的和以其它方式知晓的材料如铝酸钙、二氧化硅和氧化铝(其与一种或多种金属氧化物比如氧化钙、氧化锶和氧化钠混合)。
图4为图1的液体燃料CPOX重整器的歧管120以及相关的包含钙钛矿的管式CPOX反应器单元408的一段的放大的纵截面图。如图4中所示，歧管426的歧管段450包括上部壳(housing)结构455、下部壳结构456、歧管室429、气态CPOX反应混合物(气体)分布器427以及与管式CPOX反应器单元408的入口431气流连通的气体分布器出口430。管式CPOX反应器单元408的入口端457牢固地座落于形成于上部壳结构455内的空穴(cavity)458内并且通过O-环垫圈459与其以气密关系接合。经加热的气态CPOX反应混合物流动通过气体分布器427的出口430，通过管式CPOX反应器单元408的入口431并且进入到CPOX反应区409中，在CPOX反应区409中所述气态CPOX反应混合物经历向富含氢气的、包含一氧化碳的流出物重整物的气相CPOX转化，所述重整物在反应器单元的出口端460处通过相关的出口454离开所述反应器单元。
如下也在本发明的范围内：引入本发明的重整器作为管式固体氧化物燃料电池(SOFC)的重整部件，从而提供内部重整(IRSOFC)。一种这样的IRSOFC示于图5中。如其中所示，并且当从其最外表面到最内表面描述时，IRSOFC50包括阴极部件51、中间的电解质部件52、阳极部件53和限定通道CPOX反应区55的包含钙钛矿的重整器部件54。进入通道55的气态CPOX燃料-空气反应混合物在重整器部件54内经历CPOX重整，从而将富含氢气的重整物供应至相邻的阳极部件53，以氢气为燃料的IRSOFC以已知方式操作以产生电流。
根据本教导，本领域技术人员在考虑本文中所述的重整器的多种实施方式以及其操作原理的情况下，通过采用惯常的实验程序，可容易地优化期望的可重整燃料转化本领的具体重整器的设计、结构特性、和机械性质。
本教导涵盖以其它具体形式的实施方式而不背离其精神或本质特性。因此，前述实施方式在所有方面均应被认为是说明性的而不是对本文中描述的教导进行限制。本发明的范围因此由所附权利要求而不是前述描述所指示，并且进入到权利要求的等同的含义和范围内的所有变化都意图被包含在其中。

Claims (21)

1.重整器，其包括至少一个重整器反应器单元，所述重整器反应器单元具有：拥有外表面和内表面的限制空间的壁，所述壁的至少一段以及由其限制的空间限定重整反应区；用于将气态重整反应物的流接纳至所述重整反应区的入口端和相关的入口；用于使在所述重整反应区中制造的富含氢气的重整物流出的出口端和相关的出口，所述壁的至少的与所述重整反应区对应的那段包括钙钛矿作为其结构组分，这样的壁段是透气性的以容许气态重整反应物在其中扩散和富含氢气的重整物从其扩散。
2.权利要求1的重整器，其为催化重整器，所述钙钛矿还作为重整催化剂。
3.权利要求1-2任一项的重整器，其为CPOX重整器，所述钙钛矿还作为CPOX催化剂。
4.权利要求1-3任一项的重整器，其包括多个重整器反应器单元，各反应器单元具有限定开放的气流通道的管式构型。
5.权利要求1-4任一项的重整器，其包括多个催化重整器反应器单元，各反应器单元具有限定开放的气流通道的管式构型，所述钙钛矿还作为重整催化剂。
6.权利要求1-5任一项的重整器，其包括多个CPOX重整器反应器单元，各反应器单元具有限定开放的气流通道的管式构型，钙钛矿还作为CPOX催化剂。
7.权利要求1-6任一项的重整器，其中钙钛矿占所述壁的至少的与所述重整反应区对应的那段的结构的至少20重量％。
8.权利要求1-7任一项的重整器，其中钙钛矿占所述壁的至少的与所述重整反应区对应的那段的结构的至少50重量％。
9.权利要求1-8任一项的重整器，其中钙钛矿占所述壁的至少的与所述重整反应区对应的那段的结构的80-100重量％。
10.权利要求1-9任一项的重整器，其中所述壁的至少的与所述重整反应区对应的那段包括至少一种选自如下的组分：不同于钙钛矿的重整催化剂、金属、陶瓷、和耐高温粘合剂。
11.权利要求1-10任一项的重整器，其中氢气阻挡物附着至所述壁的至少的与所述重整反应区对应的那段的外表面。
12.权利要求1-11任一项的重整器，其中氢气阻挡物附着至所述壁的至少的与所述重整反应区对应的那段的外表面。
13.权利要求1-12任一项的重整器，其中氢气阻挡物附着至各重整器反应器的壁的至少的与其重整反应区对应的那段的外表面。
14.权利要求1-13任一项的重整器，其中氢气阻挡物附着至各重整器反应器单元的壁的至少的与其重整反应区对应的那段的外表面。
15.权利要求1-14任一项的重整器，其中氢气阻挡物附着至各重整器反应器单元的壁的至少的与其重整反应区对应的那段的外表面。
16.权利要求1-15任一项的重整器，其中氢气阻挡物附着至各重整器反应器单元的壁的至少的与其重整反应区对应的那段的外表面。
17.权利要求1-16任一项的重整器，其中所述钙钛矿为选自如下的至少一员：LaNiO3、LaCoO3、LaCrO3、LaFeO3和LaMnO3。
18.权利要求1-17任一项的重整器，其中所述钙钛矿重整催化剂为选自如下的至少一员：La1-xCexFe2O3、LaCr1-yRuyO3、La1-xSrxAl1-yRuyO3和La1-xSrxFe2O3，其中x和y为范围0.01-0.5的数。
19.权利要求1-18任一项的重整器，其中所述钙钛矿为选自如下的至少一员：锰酸锶镧、铁酸锶镧、铁酸钴锶镧、锰酸钙镧、铬酸锶镧和镓锰酸锶镧。
20.权利要求1-19任一项的重整器，其中CPOX重整器反应器单元划分成两个区域：第一区域从所述反应器单元的入口延伸至其CPOX反应区并且基本上没有重整催化剂，第二区域从它与第一区域的边界延伸至所述反应器单元的出口或者附近，其中仅有它的与所述CPOX反应区对应的壁段包括钙钛矿作为其结构组分。
21.权利要求1-20任一项的重整器，其为具有如下的管式固体氧化物燃料电池：阳极部件、电解质部件、阴极部件以及与所述阳极部件相邻的重整器部件。
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