CN101005142A - 燃料重整系统和包括燃料重整系统的燃料电池系统 - Google Patents

燃料重整系统和包括燃料重整系统的燃料电池系统 Download PDF

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CN101005142A
CN101005142A CNA2007100024379A CN200710002437A CN101005142A CN 101005142 A CN101005142 A CN 101005142A CN A2007100024379 A CNA2007100024379 A CN A2007100024379A CN 200710002437 A CN200710002437 A CN 200710002437A CN 101005142 A CN101005142 A CN 101005142A
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fuel
carbon monoxide
thermal source
reformer
hydrogen
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CN100521344C (zh
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金周龙
李圣哲
李赞镐
徐东明
金镇圹
安镇九
李东旭
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Samsung SDI Co Ltd
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Abstract

本发明提供一种燃料重整系统和包括该燃料重整系统的燃料电池系统。该燃料重整系统包括：燃料重整器，其适于由含氢燃料生成以氢为主要组分的重整气体；一氧化碳(CO)去除器，其适于从所述重整气体中去除一氧化碳；热源，其适于将热能供给到所述重整器和所述CO去除器；和移动单元，其适于将所述热源在所述燃料重整器与所述CO去除器之间移动。根据这种结构，所述燃料重整器和所述CO去除器能够通过热源被直接加热。于是，当所述CO去除器的温度达到催化剂激活温度时，所述热源能够被移动以仅对所述燃料重整器进行直接加热，从而提高了燃料重整系统的重整效果和发电效率。

Description

燃料重整系统和包括燃料重整系统的燃料电池系统
相关申请的交叉引用
本申请要求对在2006年1月17日提交到韩国知识产权局且申请号为10-2006-0005088的韩国专利申请的优先权和权益，该申请的全部内容被合并于此作为引用参考。
技术领域
本发明涉及用于重整燃料(例如，丁烷)并生成富含氢的重整气体的燃料重整系统，以及包括该燃料重整系统的燃料电池系统，更具体地说，涉及这样一种燃料重整系统和包括该燃料重整系统的燃料电池系统，在其中，热源是可移动的以将热能提供到反应区域，而用于生成以氢为基本成分的重整气体。
背景技术
燃料电池系统通过氧气与氢气之间或氧气与重整气体(富含氢)之间的电化学反应而产生电能。重整气体是从含氢燃料中获取的，而含氢燃料包括诸如甲醇、乙醇之类的醇类燃料，诸如甲烷、丙烷、丁烷之类的烃类燃料，或者诸如液化天然气之类的天然气燃料。
根据所用的电解液的种类，燃料电池系统可分为磷酸燃料电池(PAFC)、熔融碳燃料电池(MCFC)、固态氧化物燃料电池(SOFC)、聚合物电解液膜燃料电池(PEMFC)，以及碱性燃料电池(AFC)等。此外，根据燃料种类、驱动温度、输出范围等，燃料电池系统可应用于诸如移动设备、运输设备、分布式电源之类的各种领域。
近来，已经开发出一种燃料电池系统，其使用存储于市场上标准的便携式容器中的丁烷作为燃料源。
参照图6，在美国专利6,183,895中公开了这种燃料电池系统的示例。在此，该燃料电池系统包括：燃料供给装置11，其具有容纳丁烷气体的便携式压力容器1，以及适于调节丁烷气体量并控制丁烷气体流量的部件2(压力容器接收器)和部件3(蒸发器)；重整器4，其使用存储于压力容器1中的一部分丁烷气体作为燃烧室的燃料气体，并且将另一部分丁烷气体与水反应以生成包含富氢气体的重整气体；适于减少重整气体中一氧化碳浓度的一氧化碳(CO)去除器5；利用重整气体中的氢和空气中的氧来产生电的燃料电池6；以及执行直流到直流或直流到交流的稳定转换的转换器21。不过，在这种燃料电池系统的重整器4中，用于从丁烷气体中获取富含氢重整气体的重整器4的反应区域，并未被有效加热，从而导致相对较低的重整效率。
参照图7，在美国专利6,413,479中公开了一种重整器。在此，该重整器包括：原材料重整器部件，其从热源直接接收反应热来对要重整燃料进行蒸汽重整，从而生成富含氢的重整气体；以及转移反应部件和一氧化碳氧化部件，其均通过从热源传输的电热进行间接加热。不过，在这种重整器中，转移反应部件被间接加热，从而使其需要相对较长的时间来供给反应过程所需的足够热量。
发明内容
因此，本发明的一个方面在于提供这样一种燃料重整系统，其中，燃料重整器(例如重整反应单元或燃料重整部件)和转移反应部件从丁烷气体(其一氧化碳含量低)获取富含氢的重整气体。在此，燃料重整器和转移反应部件由热源直接加热，此后，当转移反应部件达到其催化剂激活温度时，热源被移动而仅对燃料重整器进行直接加热(或者热源被移动而朝向燃料重整器)，从而提高了重整效果。
本发明的另一方面在于提供这样一种包括燃料重整系统的燃料电池系统，其中，燃料重整器的反应区域和转移反应部件的反应区域在最初由热源直接加热，而当转移反应部件的反应区域达到其催化剂激活温度(或预定的催化激活温度)时，热源被移动而仅对燃料重整器的反应区域进行直接加热(或者热源被移动而朝向燃料重整器的反应区域)。
本发明的一个实施例提供一种燃料重整系统，该系统包括：燃料重整器，其适于由含氢燃料生成以氢作为主要组分的重整气体；一氧化碳去除器，其适于从所述重整气体中去除一氧化碳；热源，其适于将热能供给到所述燃料重整器和所述一氧化碳去除器；和移动单元，其适于将所述热源在所述燃料重整器与所述一氧化碳去除器之间移动。根据这种结构，燃料重整器和一氧化碳去除器能够由热源直接加热。此后，当一氧化碳去除器达到其催化剂激活温度时，热源能够被移动而仅对燃料重整器进行直接加热，从而提高了燃料重整系统的重整效果和发电效率。
根据本发明的一个实施例，所述一氧化碳去除器包括：具有转移催化剂的转移反应单元，该转移反应单元适于通过水气转移反应来减少所述重整气体中的一氧化碳浓度；和具有氧化催化剂的一氧化碳氧化单元，该一氧化碳氧化单元适于选择性地氧化和去除一氧化碳。进一步地，在一个实施例中，当所述转移反应单元被加热以达到所述转移催化剂的激活温度时，所述热源移动而朝向所述燃料重整器。
根据本发明的一个实施例，所述燃料重整系统进一步包括具有容纳空间的壳体，该壳体适于容纳所述燃料重整器和所述转移反应单元，所述热源被置于所述转移反应单元之后(或其后侧)，并将所述热源的火焰朝向所述壳体中的所述燃料重整器。进一步地，在一个实施例中，所述壳体的容纳空间中具有汽化器，该汽化器以所述火焰的方向被置于所述燃料重整器之前。
本发明的另一个实施例提供一种燃料电池系统，该系统包括：供给源，其适于供给含氢燃料；重整器，其适于重整来自所述供给源的所述含氢燃料；发电装置，其适于通过所述重整气体与氧化剂之间的电化学反应来产生电；其中，所述重整器包括：燃料重整器，其适于由所述含氢燃料生成以氢作为主要组分的重整气体；一氧化碳去除器，其适于从所述重整气体中去除一氧化碳；热源，其适于将热能供给到所述燃料重整器和所述一氧化碳去除器；和移动单元，其适于将所述热源在所述燃料重整器与所述一氧化碳去除器之间移动。
根据本发明的一个实施例，所述供给源包括丁烷气体压力容器。进一步地，在一个实施例中，所述一氧化碳去除器包括：具有转移催化剂的转移反应单元，该转移反应单元适于通过水气转移反应来减少所述重整气体中的一氧化碳浓度；和具有氧化催化剂的一氧化碳氧化单元，该一氧化碳氧化单元适于选择性地氧化和去除一氧化碳。而且，在一个实施例中，当所述转移反应单元被加热以达到所述转移催化剂的激活温度时，所述热源移动而朝向所述燃料重整器。
附图说明
下文中将根据附图以及本申请的公开内容描述本发明的示范性实施例，并结合说明书中的内容来说明本发明的原理，在附图中：
图1为根据本发明实施例的具有燃料重整系统的燃料电池系统的示意图；
图2示出图1的燃料电池系统中的可移动热源；
图3为根据本发明实施例的燃料重整系统的示意图；
图4示出图3的燃料重整系统中的可移动热源；
图5为用于移动热源的驱动单元的结构图；
图6示出常规的燃料电池系统；和
图7示出常规的重整器。
具体实施方式
在下面的详细描述中，仅通过图示显示和描述了本发明特定的示范性实施例。对于本领域技术人员应认识到的是，所描述的示范性实施例可按照不同的方式进行修改，而不偏离本发明的精神和保护范围。相应地，其中的附图和描述实际上应被认为是说明性的，而非限制性的。
在下面的实施例中，将描述以丁烷为主要组分的含氢燃料，不过本发明并不局限于此。一部分含氢燃料被用作重整燃料，以与水一起被重整并被使用，而另一部分燃料被用作燃烧燃料，用于供给热能以对重整反应单元和一氧化碳去除器进行加热，直到它们分别达到催化激活温度。进一步地，含氧空气或存储于分立的存储机构中的纯氧能够用作氧化剂。在下文中，外部空气中所含的氧被描述为氧化剂。
参照图1，燃料电池系统包括：适于供给具有丁烷基的含氢燃料的供给源10，适于重整来自供给源10的含氢燃料以生成重整气体(或富氢气体)的重整器20，和适于通过氢与氧之间的电化学反应来产生电的电池堆(stack)30。在此，空气进给器40适于将诸如空气的氧化剂供给到热源28、选择性氧化单元26和电池堆30。进一步地，回收单元50适于回收电池堆30中所生成的水。
参照图3，供给源10可包括(或者为)通用的丁烷气体压力容器10′。在如图3中所示的一个实施例中，供给源10连接到(或包括)汽化器12，该汽化器适于汽化从丁烷气体压力容器10′供给的丁烷。汽化器12通过减小压力或者通过来自热源28的热能来汽化丁烷(将在下文中进行更详细的描述)。
重整器20包括重整反应单元(或者燃料重整器或燃料重整部件)22，其适于通过由供给源10供给的重整燃料(或含氢燃料)来生成以氢为主要组分的重整气体；一氧化碳去除器，其与重整反应单元22连通并适于从重整气体中去除一氧化碳；和热源28，其适于将热能供给到重整反应单元22和一氧化碳去除器。
重整反应单元22被供给以重整催化剂22a。
重整反应单元22通过蒸汽重整(SR)方法、自动热重整(ATR)方法和部分氧化(POX)方法等来重整含氢燃料，不过本发明并不局限于此。部分氧化方法和自动热重整方法对于初始启动和负载变化具有相对较好的响应特性，而蒸汽重整方法对于生成氢气具有相对较高的效率。蒸汽重整方法通过化学反应，即含氢燃料与蒸汽之间的在催化剂上的吸热反应，来生成富含氢的重整气体。在此，应使用蒸汽重整方法，这是因为，即使进行所述吸热反应需要相对较多的能量，但可稳定地生成重整气体并获得相对较高的氢浓度。因此，在一个实施例中，使用蒸汽重整方法。例如，在重整反应单元22采用蒸汽重整方法的情况下，从供给源10供给的重整燃料(即具有丁烷基的含氢燃料)之间的蒸汽重整反应(即指下面的反应式1)在重整催化剂22a上进行，而在重整催化剂22a上产生的水通过回收单元50被回收，从而生成富氢的重整气体。
反应式1：
n-C4H10+8H2O4CO2+13H2，ΔH298＝485.3KJ/mol
重整催化剂22a可包括载体及其载带的金属，如钌、铑、镍等。该载体可包括二氧化锆、氧化铝、硅胶、活性氧化铝、二氧化钛、沸石、活性碳等。前述的重整气体可包括少量的二氧化碳、甲烷和一氧化碳。特别地是，一氧化碳毒化可用于电池堆30的电极的铂催化剂，并使燃料电池系统的性能恶化。因此，应从前述的重整气体中去除一氧化碳。
为去除一氧化碳，所述一氧化碳去除器包括：进行水气转移反应的水气转移单元24，和进行选择性氧化催化反应的选择性氧化单元26。水气转移单元24具有转移催化剂24a，而选择性氧化单元26具有氧化催化剂26a。进一步地，选择性氧化反应所需的诸如氧气的氧化剂，其通过空气进给器40而供给到选择性氧化单元26。水气转移反应和选择性氧化催化反应可分别被表示为下面的反应式2和3。
反应式2：
CO+H2OCO2+H2，ΔH298＝-41.1KJ/mol
反应式3：
CO+1/2O2CO2+13H2，ΔH298＝-284.1KJ/mol
此外，重整器20被提供以热源28，该热源28使用来自供给源10的丁烷作为燃烧燃料。热源28被供给以来自空气进给器40的诸如氧气的氧化剂。在此，热源28将加热所需的热能供给到重整器20的重整反应单元22、水气转移单元24和选择性氧化单元26，以分别达到催化剂激活温度。
参照图3，重整器20包括形成有容纳空间的壳体20a，该壳体20a具有特定的或预定的规格以分别在其中容纳重整反应单元22和水气转移单元24。热源28被置于水气转移单元24之后(或处于其后侧)，使得来自热源28的火焰28a朝向所述容纳空间。在一个实施例中，汽化器12被连通地置于供给源10(例如丁烷气体压力容器10′)与重整反应单元22之间。汽化器12汽化从丁烷气体压力容器10′供给的重整燃料。在热源28中，燃烧反应可以被表示为下面的反应式4。
反应式4：
n-C4H10+6.5O24CO2+5H2O，ΔH298＝-2658.5KJ/mol
更详细地说，一部分丁烷气体作为燃烧燃料而从丁烷气体压力容器10′被供给到热源28，而另一部分丁烷气体则作为重整燃料被供给到汽化器12。在此，热源28被进给以来自空气进给器40的氧气，而汽化器12被供给以水。一些丁烷气体，即供给到热源28的燃烧燃料，通过基于前述反应式4的反应而被燃烧，而此处产生的热能被传输到重整反应单元22和水气转移单元24。在一个实施例中，来自热源28的火焰28a接触水气转移单元24，从而将热能直接传输到水气转移单元24。
当水气转移单元24通过热源28的火焰28a被加热而达到转移催化剂24a(例如，铜-锌催化剂)的激活温度而且此后水气转移单元24的温度由温度传感器(或被称为第二温度传感器)24b被检测时，第二温度传感器24b向控制器提供水气转移单元24的温度的相关信息，如图5中所示。之后，如图5中进一步所示，控制器驱动一驱动马达，以如图2和图4中所示的将热源28移动而朝向重整反应单元22。这样，如图1和图3中所示，水气转移单元24由热源28的火焰28a直接加热，以减少加热水气转移单元24所需的加热时间，直到达到转移催化剂24a的激活温度。
进一步地，如图2和图4所示，热源28移动而朝向重整反应单元22之后，热源28的火焰28a直接接触并加热重整反应单元22。在此，被设置在重整反应单元22中的温度传感器(或称为第一温度传感器)22b，实时检测重整反应单元22的温度。
当重整反应单元22的温度达到了重整催化剂22a的激活温度时，第一温度传感器22b向控制器提供此加热状态，因而，控制器减少所供给的燃烧燃料的量(或减少燃烧燃料的供给量)，从而减小来自热源28的火焰28a的尺寸。
而且，热源28移向重整反应部件22，而水气转移单元24的加热状态通过沿壳体20a内壁的回放热(或回返热)而被间接地保持。进一步地，当由第二温度传感器24b所检测到的水气转移单元24的温度低于转移催化剂24a的激活温度时，控制器控制驱动马达，以将热源28返回移动而朝向水气转移单元24。
在重整反应部件22和水气转移单元24通过热源28被加热而达到各自的催化剂激活温度的情况下，重整燃料，即从丁烷气体压力容器10′供给的丁烷气体，在通过汽化器12时与水一起被汽化。之后，被汽化的重整燃料在通过重整反应单元22时基于反应式1进行反应，从而生成富含氢的重整气体(或以氢为基本成分的重整气体)。
当重整气体通过水气转移单元24时，一氧化碳通过反应式2而被从重整气体中去除，从而导致重整气体中所包含的一氧化碳的第一减量。为了进一步减少重整气体中所包含的一氧化碳的量以达到最终浓度水平，例如至少达到10ppm或更低，选择性氧化单元26被连通到水气转移单元24的后部。
选择性氧化单元26具有氧化催化剂26a。
举例来说，氧化催化剂26a包括铂催化剂或钌催化剂，并可具有固态形式或多孔形式。因此，在通过水气转移单元24之后，当通过选择性氧化单元26的氧化催化剂26a时，更多的一氧化碳通过反应式3而被从重整气体申去除，从而生成一种具有接近于高氢纯度的富氢气体。
参照图1和图2，这样的富氢气体被供给到电池堆30。也就是说，当富氢气体和空气被供给到电池堆30的阳极电极和阴极电极时，通过氢的氧化反应而产生的电，通过集电器(未示出)而被供给到外部电路。
更详细地说，由重整器20的选择性氧化单元26生成的高纯度的氢气，被供给到电池堆30的阳极电极(未示出)，而含氧空气从空气进给器40被供给到电池堆30的阴极电极(未示出)。进一步地，氢离子通过电池堆30的MEA(未示出)进行传输，通过氢气与氧气之间的化学反应来产生电。而且，基于电池堆30中的化学反应而生成的水，被回收到回收单元50并被再利用。
根据本发明的实施例，用于从丁烷气体(其中的一氧化碳含量低)获取富含氢重整气体(即其中具有充足的氢)的燃料重整部件和转移反应部件，通过热源而被直接加热。此后，当转移反应部件的温度达到催化剂激活温度时，热源被移动而仅对燃料重整部件进行直接加热(例如，热源被移动而朝向燃料重整部件)，从而提高了燃料重整系统的重整效果。
进一步地，根据本发明的实施例，当转移反应单元的反应区域被加热而达到催化剂激活温度(或预定的催化剂激活温度)而且燃料重整部件的反应区域和转移反应部件的反应区域通过来自热源的热能而被直接加热时，热源被移动而仅对燃料重整部件的反应区域进行直接加热(例如热源被移动而朝向燃料重整部件的反应区域)，从而提高了燃料电池系统的发电效率。
虽然已结合具体的示范性实施例对本发明进行了描述，不过，对于本领域技术人员而言，应理解的是，本发明并不限于所公开的实施例，而是相反地，本发明意在涵盖包括于所附权利要求书及其等同物的精神和范围之内的各种修改。

Claims (22)

1、一种燃料重整系统，包括：
燃料重整器，其适于由含氢燃料生成以氢为主要组分的重整气体；
一氧化碳去除器，其适于从所述重整气体中去除一氧化碳；
热源，其适于将热能供给到所述燃料重整器和所述一氧化碳去除器；和移动单元，其适于将所述热源在所述燃料重整器与所述一氧化碳去除器之间移动。
2、根据权利要求1所述的燃料重整系统，其中所述移动单元包括：适于移动所述热源的驱动马达，和适于控制所述驱动马达操作的控制器。
3、根据权利要求2所述的燃料重整系统，其中所述一氧化碳去除器包括：具有转移催化剂的转移反应单元，该转移反应单元适于通过水气转移反应来减少所述重整气体中一氧化碳的浓度；和具有氧化催化剂的一氧化碳氧化单元，该一氧化碳氧化单元适于选择性地氧化和去除一氧化碳。
4、根据权利要求3所述的燃料重整系统，进一步包括：具有容纳空间的壳体，该壳体适于容纳所述燃料重整器和所述转移反应单元。
5、根据权利要求4所述的燃料重整系统，其中，所述热源被置于所述转移反应单元之后，并将所述热源的火焰朝向所述壳体中的所述燃料重整器。
6、根据权利要求5所述的燃料重整系统，其中，当所述转移反应单元被加热以达到所述转移催化剂的激活温度时，所述热源移动而朝向所述燃料重整器。
7、根据权利要求6所述的燃料重整系统，其中所述转移反应单元具有温度传感器。
8、根据权利要求5所述的燃料重整系统，其中，所述壳体的容纳空间中具有汽化器，该汽化器以所述火焰的方向被置于所述燃料重整器之前并用于汽化所述含氢燃料。
9、根据权利要求2所述的燃料重整系统，其中所述燃料重整器具有温度传感器。
10、根据权利要求9所述的燃料重整系统，其中所述控制器控制将被供给到所述热源的燃烧燃料的量。
11、根据权利要求1所述的燃料重整系统，其中所述含氢燃料从液化气体容器中进行供给。
12、一种燃料电池系统，其包括：
供给源，其适于供给含氢燃料；
重整器，其适于重整来自所述供给源的所述含氢燃料；
发电装置，其适于通过所述重整气体与氧化剂之间的电化学反应来产生电；
其中，所述重整器包括：燃料重整器，其适于由含氢燃料生成以氢为主要组分的重整气体；一氧化碳去除器，其适于从所述重整气体中去除一氧化碳；热源，其适于将热能供给到所述燃料重整器和所述一氧化碳去除器；和移动单元，其适于将所述热源在所述燃料重整器与所述一氧化碳去除器之间移动。
13、根据权利要求12所述的燃料电池系统，其中所述移动单元包括：适于移动所述热源的驱动马达，和适于控制所述驱动马达操作的控制器。
14、根据权利要求13所述的燃料电池系统，其中所述一氧化碳去除器包括：具有转移催化剂的转移反应单元，该转移反应单元适于通过水气转移反应来减少所述重整气体中一氧化碳的浓度；和具有氧化催化剂的一氧化碳氧化单元，该一氧化碳氧化单元适于选择性地氧化和去除一氧化碳。
15、根据权利要求14所述的燃料电池系统，进一步包括：具有容纳空间的壳体，该壳体适于容纳所述燃料重整器和所述转移反应单元。
16、根据权利要求15所述的燃料电池系统，其中所述热源被置于所述转移反应单元之后，并将所述热源的火焰朝向所述壳体中的所述燃料重整器。
17、根据权利要求16所述的燃料电池系统，其中，当所述转移反应单元被加热以达到所述转移催化剂的激活温度时，所述热源移动而朝向所述燃料重整器。
18、根据权利要求17所述的燃料电池系统，其中所述转移反应单元具有温度传感器。
19、根据权利要求16所述的燃料电池系统，其中，所述壳体的容纳空间中具有汽化器，该汽化器以所述火焰的方向被置于所述燃料重整器之前并用于汽化所述含氢燃料。
20、根据权利要求13所述的燃料电池系统，其中所述燃料重整器具有温度传感器。
21、根据权利要求20所述的燃料电池系统，其中所述控制器控制将被供给到所述热源的燃烧燃料的量。
22、根据权利要求12所述的燃料电池系统，其中所述供给源包括液化气体容器。
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