CN1228749A - 将烃类燃料转化成氢气和二氧化碳的方法和装置 - Google Patents

将烃类燃料转化成氢气和二氧化碳的方法和装置 Download PDF

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CN1228749A
CN1228749A CN97197471A CN97197471A CN1228749A CN 1228749 A CN1228749 A CN 1228749A CN 97197471 A CN97197471 A CN 97197471A CN 97197471 A CN97197471 A CN 97197471A CN 1228749 A CN1228749 A CN 1228749A
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hydrocarbon
fuel
pipe
reactor
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CN1133578C (zh
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劳伦斯·G·克劳森
威廉姆·L·米切尔
杰弗里·M·本特利
约翰内斯·H·J·泰斯恩
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EPYX Co.
Nuwarui Ovonic Fuel Cell Co.
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Arthur D Little Inc
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Abstract

本发明公开了一种用于将烃类燃料或醇转化成氢气和二氧化碳的装置和方法。所述的装置包括具有部分氧化反应区的第一级反应器和分开的与部分氧化反应区不同的蒸汽转化反应区。所述的第一级反应器具有在部分氧化反应区处的第一级反应器入口和在蒸汽转化区处的第一级反应器的出口。所述的烃水蒸汽转化装置还包括延伸在第一级反应器周围的螺旋管。所述的螺旋管具有连于氧源的第一端口和在部分氧化反应区处连于第一级反应器的第二端口。来自含氧源的氧气可通过螺旋管导入至第一级反应器。具有第二级反应器入口和第二级反应器出口的第二级反应器环绕布置在第一级反应器周围,所述的螺旋管布置在第一级反应器和第二级反应器之间,且来自第一级反应器的气体可被导入通过第二级反应器。

Description

将烃类燃料转化成氢气和二氧化碳的方法和装置
燃料电池在固定物和运输业应用中产生动力方面继续起着日益增长的重要作用。燃料电池的主要优点是它可以高效运行，它不同于目前使用的热发动机，它不受Carnot循环效率限制。而且，在操作纯净方面，燃料电池远胜于任何已知的能量转换装置。燃料电池是化学能源，由一种还原剂(氢)和一种氧化剂(氧)之间的化学反应产生电能，氢和氧以与能量负荷成比例的速率加入到电池中。因此，燃料电池需要氧气和一个氢源来运行。
现在有两个问题限制了氢气的使用。第一，氢气(H2)与普通的烃相比有一个较低的体积能量密度，这就意味着与用普通的烃贮存相同数量的能量相比，用氢贮存时将占有更大的体积。第二，目前没有能够支持大量燃料电池的能量系统所需的分布广泛的氢基础设施。
在各种烃类和醇类燃料的分子结构中含有能够供给燃料电池动力的吸引人的氢源。一种烃水蒸汽转化装置是一种裂解初始燃料的分子产生能够供给燃料电池动力的富氢气体流的装置。尽管转化烃类和醇类燃料的工艺已经在大的工业基础上建立起来，但在小规模、高度完整的装置上类似的发展还未见报道。
因此，需要一种更小型的装置，用于从各种烃类燃料源中产生氢气，用于燃料电池以供给车辆动力。
本发明涉及一种用于将醇类或烃类燃料转化成氢气和二氧化碳的烃水蒸汽转化装置和方法。
该烃水蒸汽转化装置包括第一级反应器，其具有部分氧化反应区和与部分氧化反应区不同的、分开的蒸汽转化反应区。该第一级反应器具有在部分反应区处的第一级反应器入口，和在蒸汽转化区处的第一级反应器出口。该烃水蒸汽转化装置还包括延伸在第一级反应器周围的螺旋管。该螺旋管具有连于含氧源上的第一端口，和在部分氧化反应区处连于第一级反应器上的第二端口。来自含氧源的氧气可通过螺旋管导入至第一级反应器中。具有第二级反应器入口和第二级反应器出口的第二级反应器环状地布置在第一级反应器周围。螺旋管布置在第一级反应器和第二级反应器之间，且来自第一级反应器的气体可被导入通过第二级反应器。
该方法包括通过布置在第一级反应器周围的螺旋管导入含氧气体。将烃蒸气和水蒸汽导入至螺旋管以形成氧气、燃料蒸气和水蒸汽的混合物。该氧气、燃料蒸气和水蒸汽的混合物导入至第一级反应器中。燃料蒸气自发地部分氧化形成热的含有一氧化碳和氢气的转化产物物流。剩余的燃料蒸气在热的转化产物物流中进行水蒸汽转化形成氢气和一氧化碳。热的转化产物物流被导入通过螺旋管的外部，在此，热的转化产物物流加热螺旋管内部的混合物。转化产物物流的部分一氧化碳气体通过高温转化反应转化成二氧化碳和氢气。至少一部分转化产物物流中的剩余的一氧化碳气体通过低温转化反应转化成二氧化碳和氢气。
在另一用于将烃类燃料转化成氢气和二氧化碳的烃水蒸汽转化装置的实施方案中，该装置包括：第一级管，其具有用于接收含氧气体和第一级燃料的第一级混合物的第一级管入口，此混合物可以是烃或醇，和用于导入第一级混合物的第一级反应转化产物的第一级管出口。第二级管环绕布置在第一级管周围，其中第二级管具有用于接收第二级燃料的第二级混合物的第二级管入口，此混合物可以是烃或醇，和水蒸汽。第二级管具有用于导入第二级混合物的第二级反应转化产物的第二级管出口。催化转化区环状地布置在第二级管周围。第一级反应转化产物和第二级反应转化产物能够通过第一级管出口和第二级管出口分别导入至用于进一步转化该混合物的催化转化区。在优选的实施方案中，烃类燃料分馏器连接在第一级管入口和第二级管入口处。此分馏器能够从烃类燃料中分离出重组分，其后续导入至第一级管中的部分氧化区；可从烃类燃料中分离出轻组分，其后续导入至第二级管中的蒸汽转化区。
在用于将烃类或醇类燃料转化成氢气和二氧化碳的方法的另一实施方案中，将第一级烃类或醇类燃料和含氧气体的第一级混合物导入至第一级管中。在第一级混合物的烃类或醇类燃料自发地部分氧化形成第一级热的含有氢气和一氧化碳的转化产物物流。第二级烃类或醇类燃料和水蒸汽的第二级混合物导入至环绕布置在第一级管周围的第二级管中。第二级混合物的第二级烃类或醇类燃料的部分水蒸汽转化形成第二级热的含有氢气和一氧化碳的转化产物物流。第一级热的转化产物物流和第二级热的转化产物物流通入到催化转化区使这些转化产物物流进一步转化成氢气和二氧化碳。在优选的实施方案中，在导入至第一级管和第二级管之前的烃类燃料被分馏成烃类燃料的重组分和烃类燃料的轻组分。重组分随后导入至部分氧化区。轻组分导入至蒸汽转化区。
本发明有许多优点。本发明的装置能使用各种烃类燃料，如汽油、JP-8、甲醇和乙醇。部分氧化反应区允许燃料部分燃烧而不形成烟灰，而且给环绕在部分氧化区周围的水蒸汽转化区和反应器的其他部分提供热量。而且，本装置足够小，以致可供汽车使用。在一些实施方案中，装置中包括一种高温转化催化剂，此催化剂与只使用低温转化催化剂相比可使装置更小、重量更轻。
图1是本发明装置的第一种实施方案的正投影侧面图；
图2是本发明装置的第二种实施方案的正投影侧面图；
图3是本发明装置的第三种实施方案的正投影侧面图。
本发明方法和装置的特征和详细说明现在将参照附图更详细地描述并在权利要求中指出。出现在不同附图中的相同数字代表相同的项目。应该知道，本发明特定的实施方案通过实例来表明，但这并不作为本发明的限制。在各种实施方案中能够具有本发明的主要特征而不背离本发明的范围。除非另有说明，所有百分数和分数都以重量计。
图1显示了本发明的一种实施方案。烃水蒸汽转化装置10具有转化反应器12。转化反应器12可以是圆柱型的。烃水蒸汽转化装置10具有上部分14和下部分16。设置在转化反应器12中心的是第一级反应器18，它充分地扩大了转化反应器12的高度。第一级反应器18具有第一级反应器入口20，用于接收气体进入第一级反应器18，并且能成切线导入气体通过第一级反应器。在烃水蒸汽转化装置10上部14，第一级反应器18具有第一级反应器出口22，用于气体离开第一级反应器。多孔板31位于第一级反应器出口22处，并且覆盖第一级反应器18的横断面。部分氧化反应区24是在第一级反应器18的下部16内。
部分氧化反应区24适合于烃类或醇类燃料与氧部分氧化以形成一种含有一氧化碳、水蒸汽和氢气的混合物。水蒸汽转化区26是在部分氧化区24的上部，内含有水蒸汽转化催化剂28。优选的是，水蒸汽转化催化剂包括镍和一定量的贵金属，如钴、铂、钯、铑、钌、铱，和一种载体，如氧化镁、铝酸镁、氧化铝、二氧化硅和氧化锆，它们可以单独或结合起来使用。作为一种选择，水蒸汽转化催化剂28可以是如镍的单一金属，载于一种耐热的载体上，所述载体如氧化镁、铝酸镁、氧化铝、二氧化硅和氧化锆，它们可以单独或结合起来使用，可由一种如钾的碱金属助催化。蒸汽转化区26能自热地将水蒸汽和在部分氧化区24产生的甲烷转化成氢气和一氧化碳。蒸汽转化催化剂28可以是粒状的，由多孔板30和多孔板31载于部分氧化区24中。
螺旋管32延伸了第一级反应器18的长度。螺旋管32的第一端口34位于入口室33处。氧源42通过导管35连到带有第一端口入口36的入口室33，用于接收来自氧气区40的含氧气体。螺旋管32的第二端口44连到第一级反应器入口20上。合适的含氧气体的例子包括氧气(O2)和空气等。燃料入口46连到距第二端口44最近的螺旋管32上。导管50从燃料源48延伸到燃料入口46。合适燃料的例子包括烃类，也包括醇在内。燃料包括汽油、煤油、JP-8、甲烷、甲醇和乙醇。水蒸汽入口52挨近燃料入口46。水蒸汽从蒸汽源54引入到蒸汽管56中，通过第一级水蒸汽入口52进入螺旋管32。在另一实施方案中，燃料和水蒸汽可以导入螺旋管32。
第二级反应器58环状地布置在第一级反应器18的周围。第二级反应器入口60接收来自第一级反应器出口22的气态产物。在烃水蒸汽转化装置10底部16的第二级反应器出口62允许气体离开第二级反应器58。螺旋管32布置在第一级反应器18和第二级反应器58之间，来自第一级反应器18的气体能够从第二级反应器入口60，经螺旋管32的周围进入第二级反应器58，到达第二级反应器出口62。气流分配区63使来自第二级反应器出口62的气体到达高温转化区64。额外的水蒸汽或水能够从一个水蒸汽源通过第二个水蒸汽入口53导入至第二级反应器58，用以提供更多的水蒸汽去供给附加的冷却和燃料的进一步转化。
高温转化区64环状地位于第二级反应器58和转化反应器12之间，并且含有高温转化催化剂。合适的高温转化催化剂的例子是在约300℃至约600℃温度范围之间的某一温度下可操作的催化剂。优选的高温转化催化剂包括过渡金属氧化物，如三价铁的氧化物(Fe2O3)和三价铬的氧化物(Cr2O3)。其他类型的高温转化催化剂包括氧化铁和氧化铬，用下列物质助催化，如铜、铁的硅化物、载体上的铂、载体上的钯、和其他载体上的铂族金属，它们可单独或结合起来使用。高温转化催化剂66通过多孔板68和多孔板70固定于适当的位置。气体能通过高温转化区64，经过多孔板70进入到脱硫区71。
在高温转化区64上部是脱硫区71。脱硫区71内含有一种能降低气体物流中对低温转化催化剂有害的硫化氢(H2S)含量的催化剂，此催化剂可使硫化氢的浓度降至约百万分之一或更小。一种合适的催化剂的例子包括氧化锌。脱硫区71的大小依所用燃料的类型而定。如果使用低硫燃料，就需要小的脱硫区。如果使用高硫燃料，一个较大的脱硫区是必须的。气体能够经过多孔板73通过脱硫区71，到达冷却区72。
冷却区72包括许多垂直的翅片74，这些翅片把热量从第二级反应器58发散到转化反应器12中，它从高温转化区64扩展到低温转化区76。
冷却管78螺旋状绕在第二级反应器58周围，并连到垂直翅片74上。冷却管78具有冷却管入口80，用于接收冷却介质，如水，通过冷却管78至冷却管出口82。在另一实施方案中，冷却管78在第二级反应器58周围再次缠绕。来自高温催化剂区64的气体产物能够在垂直翅片74间通过，并通过冷却管78使气体产物冷却。
低温转换区76环绕在冷却区78上部并在第二级反应器58和转化反应器12之间，并且包括低温转化改性催化剂84，用以减少一氧化碳至小于1％水平，或更低(以体积计)。一种合适的低温改性催化剂的例子是可操作温度在约150℃至约300℃之间的某一温度下。优选此低温改性催化剂包括氧化铜(CuO)和氧化锌(ZnO)。其他类型的低温转化催化剂包括载于其他过渡金属氧化物如氧化锆上的铜，载于过渡金属氧化物或耐火载体如二氧化硅或氧化铝上的锌，载体上的铂、载体上的铼、载体上的钯、载体上的铑和金。低温转换区催化剂84由下部的多孔板86和上部多孔板88固定于适当的位置。来自冷却区72的气体产物能够经过孔板86通过低温转换区76直至上部孔板88。出口区90在低温转换区76上部并有转化出口92。
在将烃类燃料转化为氢气的方法中，含氧气体，如空气，通过导管35从氧源42导入入口室33至氧气区40进入垂直管线32的第一端口入口36。烃水蒸汽转化装置10可以在压力范围约0至500psig(表压，磅/英寸2)间操作。含氧气体，如空气，被预热至约450℃。在优选的实施方案中，空气流速高于约每秒40米。
合适的烃类或醇类蒸气从燃料源48通过燃料管50导入至燃料入口46。合适的烃类燃料的例子包括汽油、JP-8、甲醇、乙醇、煤油和其他合适的通常用于转化装置的烃类，气体烃类，如甲烷或丙烷也可使用。水蒸汽从蒸汽源54通过蒸汽管56导入至第一级蒸汽入口52。水蒸汽温度范围在约100℃至约150℃之间。空气、水蒸汽和烃类燃料以足以在螺旋管32中混合并自发进行部分氧化的速率加入，以使此混合物进入部分氧化区24通过第一级反应器入口20时形成包括一氧化碳和氢气的热的转化产物物流。在一个优选的实施方案中，含氧气体成切线导入部分氧化区24内部的周围，这里是一个空腔。在部分氧化区24中，转化产物可以包含甲烷、氢气、水和一氧化碳。部分氧化区24具有优选的温度范围在约950℃至约1150℃。一种更重的燃料优选运行在此温度范围的较高一端，而一种较轻的燃料运行在此温度范围的较低一端。
转化产物自部分氧化区24通过多孔板30导入水蒸汽转化区26。在水蒸汽转化区26，来自部分氧化区24，在热的转化气流中的剩余的烃类蒸气在水蒸汽转化催化剂28存在下进行水蒸汽转化，转化成氢气和一氧化碳。水蒸汽转化区26的温度通常是在约700℃至900℃的范围内。部分氧化反应提供足够的热量以供热给螺旋管32，预热空气和螺旋管32中的其他物料，并且也供热给水蒸汽转化步骤。烃类燃料在部分氧化区24中部分然烧，水蒸汽中剩余的燃料与部分氧化区燃烧产物混合用于在水蒸汽转化催化剂28存在下水蒸汽转化并且烃类转换成一氧化碳和氢气。从水蒸汽转化区26流出的热的转化产物物流的温度在约700℃至约900℃之间。热的转化产物物流被导入至第一级反应器18和第二级反应器58，且在螺旋管32的外部周围，热的转化物流通过加热螺旋管32和第一级反应器18和第二级反应器56中的物料而得到冷却。
热的转化产物物流流出第二个反应器出口62到达气流分配区63，在此被冷却到约300℃至约600℃之间的某一温度，并经过多孔板68导入至高温转化区64，在此，在约300℃至约600℃范围内的某一温度下通过将热的转化物流与高温转化催化剂66接触而被除去几乎所有的一氧化碳或使其降低。高温转化区64是在绝热下操作以减少一氧化碳水平并伴随着适度的温升。在一种实施方案中，进入高温转化区64的热的转化物流带有14-17％(体积)的一氧化碳，而流出高温转化区64时，含有约2-4％(体积)的一氧化碳。
处理转化产物物流的高温转化区通到脱硫区71，在此，物流中的硫化氢的含量降至低于大约百万分之一(IPPM)的浓度。转化产物被从脱硫区71导入至冷却区72，在此，物流与垂直翅片74和冷却管78接触，使物流的温度降至约150℃至约300℃之间，这是由于低温转化催化剂84对温度敏感并且在高于约300℃的温度下可能会产生烧结。冷却区72为低温转化区76冷却高温转化产物气体。冷却区管78连续不断地流动操作，以保证准确和最大的蒸气侧热传递，以减少泡沫和腐蚀，允许使用污染水，并得到一个恒定的最低壁温。
转化产物物流通过多孔板86被导入至低温转化反应区76，在此转化产物物流与低温转化催化剂84相接触，使转化产物物流中剩余的一氧化碳气体的至少一部分通过低温转化反应转化成二氧化碳，形成产物物流。低温转化反应区76是在绝热下操作，以使剩余的一氧化碳量减少至痕量的水平，并伴随着适度的催化剂温度升高。生成的气体产物物流通过多孔板88从低温转化反应区76流出到尾气区90，到烃水蒸汽转化装置出口92。流出的产物物流会有这样的组成：(以湿体积计)氢气约为40％，一氧化碳低于1％。
本发明的第二种实施方案如图二所示。第二个转化装置100具有转化装置外壳102。转化装置外壳102具有上部104和下部106。装在转化装置外壳102中央部位的是第一级管108，它相当大地增加了转化装置外壳102的高度。第一级管108在低端106具有第一级管入口110，用于接收气体进入第一级管108。第一级管108是用于接收氧和第一级烃类燃料的第一级混合物。第一级管出口112是用于将第一级混合物的第一级反应转化产物导入混合区114。
第二级管116环绕在第一级管108周围。第二级管116具有第二级管入口118，用于接收第二级烃类燃料和蒸汽。第二级管116也具有第二级管出口120，用于导出第二级混合物的第二级反应转化产物。第二级管116可以包括一种水蒸汽转化催化剂，合适的催化剂的例子包括镍，一定量的贵金属，如钴、铂、钯、铑、钌、铱，和载体如氧化镁、铝酸镁、氧化铝、氧化硅和氧化锆，它们可以单独或结合起来使用。作为一种选择，水蒸汽转化催化剂可以是诸如镍等的单一金属，载于一种耐热的载体上，如氧化镁、铝酸镁、氧化铝、氧化硅或氧化锆，它们可以单独或结合起来使用，可由一种如钾的碱金属助催化。在另一种实施方案中，第二级管116可以环绕布置在第一级管108内，在此，蒸汽和燃料可以被导入中央管，并且燃料和氧可被导入环绕在中央管周围的管中。
氧源122通过氧管124与第一级管108相连。合适氧源的例子可以是氧气或空气。蒸汽源126通过蒸汽管128与第二级管116相连。在一种实施方案中，蒸汽源126可以提供蒸汽来源，其温度为约150℃，压力为约60Psig。
燃料源130经燃料管132连接到分馏器134。燃料源130包括一种合适的燃料，如烃类，包括汽油、JP-8、煤油，还有醇类，包括甲醇和乙醇。分馏器134具有轻组分出口136，用于从分馏器134导出轻组分，及重组分出口138，用于从分馏器134导出重组分。重组分可以从重组分出口138通过重组分管140导入第一级管入口110。轻组分可以从轻组分出口138通过轻组分管142导入第二级管入口118。在另一实施方案中，独立的源可以用于重组分(第一级烃类燃料)和轻组分(第二级烃类燃料)而不用分馏器。
催化转化区144环绕在第二级管116周围。第一级反应转化产物和第二级反应转化产物可以通过第一级管出口112和第二级管出口120分别导入催化转化区144上部的混合区114。
催化转化区144包含一种催化剂，用于进一步将混合物转化为氢气。一个合适的催化剂的例子包括镍、一定量的贵金属，如钴、铂、钯、铑、钌、铱，和一个载体如氧化镁、铝酸镁、氧化铝、氧化硅和氧化锆，它们可以单独或结合起来使用。作为一种选择，此催化剂可以是如镍的单一金属，载于一种耐热的载体上，如氧化镁、铝酸镁、氧化铝、氧化硅或氧化锆，它们可以单独或结合起来使用，可由一种如钾的碱金属助催化。催化转化区144的高度可基本上是第一级管108和第二级管116的长度。催化转化区144是充分多孔的，以允许从出口区146来的气体通过。催化转化区144中的催化剂147用下部多孔板148和上部多孔板150固定装载。催化转化区144中的产物气体能够从出口区146经由转化装置外壳出口152流出第二级转化装置100。
在本发明的将烃类燃料转化成氢气和二氧化碳的第二个实施方案中，一种燃料从燃料源130通过燃料管132导入分馏器中。此燃料在分馏器134中分为轻组分和重组分。重组分经重组分管140从重组分出口138导入第一级管入口110。一种含氧气体如空气，经氧管124从氧源122导入第一级管入口110。含氧气体和烃类燃料的重组分在第一级管中形成混合物，在此，第一级混合物的烃类燃料自发地发生部分氧化反应形成第一级热的含有氢气和一氧化碳的转化产物物流。第一级热的转化产物物流可以加热至约1,525℃。燃料与氧的比例依所使用的燃料类型而定。较重的燃料需要一个较高的燃烧温度。燃料的部分氧化形成含有一氧化碳、水、氢气和甲烷的燃料混合物。从部分氧化反应产生的过剩热量允许从第一级管108向第二级管116传热。通过在高于约1,375℃的温度下燃烧重组分，在部分氧化区没有明显地形成烟灰或焦油。如果需要，可以用热表面点火器或火花塞来点火。
燃料的轻组分从分馏器134的轻组分出口136导出，通过轻组分管142进入第二级管116。蒸汽从蒸汽源126导出，通过蒸汽管128，由第二级管入口118进入第二级管116。氧气也是从氧源122导出，通过氧管124，由第二级管入口118进入第二级管116。在另一个实施方案中，只有蒸汽和烃类燃料的轻组分进入第二级管。在环绕在第一级管108周围的第二级管116中形成含有含氧气体、烃类燃料的轻组分和水蒸汽的第二级混合物。第二级混合物中的烃类燃料部分反应形成包括氢气和一氧化碳的第二级热的转化产物物流。在水蒸汽的存在下，第二级混合物部分水蒸汽转化。来自第一级管108中的反应热可提供能量以帮助第二级管116中的反应进行。
自第一级管108的第一级热转化产物物流和自第二级管116的第二级热转化产物物流通过第一级管出口112和第二级管出口120，分别导入混合区114。分开的管允许碳还原操作在高燃料与氧之比约为4至1下进行，也允许使用馏出的燃料，如汽油、柴油机燃料、喷气燃料或煤油，从而重组分型燃料是优选地导入第一级管108，用于断裂大分子需要的高温燃烧，而轻组分型蒸气被导入第二级管116通过与燃烧室的热接触进行部分水蒸汽转化。第一级热转化产物物流和第二级热转化产物物流在混合区114中混合。此混合物从混合区114经催化转化区144导入到出口区146。在催化转化区144中，剩余的一氧化碳转化成二氧化碳形成产物物流。产物物流从出口区146经第二级转化装置100经转化装置外壳出口152排出。
本发明的另一实施方案示于图3。第三级转化装置200具有转化装置外壳202。转化装置外壳202具有上部204和下部206。安装在转化装置外壳202中心的是第一级管208。第一级管208在下部206具有第一级管入口210，用于接收气体进入第一级管208。第一级管208在上部204具有第一级管出口212，用于从第一级管208中放出气体。第一级管208包括水蒸汽转化催化剂214，用于在水蒸汽存在下转化烃类。合适的水蒸汽转化催化剂的实例是镍、一定数量的贵金属如钴、铂、钯、铑、钌、铱，和一种载体如氧化镁、铝酸镁、氧化铝、氧化硅和氧化锆，它们可以单独或结合起来使用。另外，水蒸汽转化催化剂可以是单一的金属，如镍，载于一种耐热的载体上，如氧化镁、铝酸镁、氧化铝、氧化硅或锆上，它们可以单独或结合使用，用一种碱金属如钾助催化。第一级管208是用于接收水蒸汽和第一级烃或醇类燃料的混合物。第一级管的出口212是用于将第一级混合物的第一级反应转化产物导入混合区216。第一级管208可以具有统一的直径，或者呈锥形，例如在第一级管入口210处的直径小于在第一级管出口212处直径。
水蒸汽源213经水蒸汽管215与第一级管208相连。蒸汽源213可以提供蒸汽源，其温度为约150℃，压力约60Psig。轻燃料源217经轻燃料管219连到第一级管208上，用于将轻燃料导入第一级管208，轻燃料包括合适的燃料，如烃，包括汽油、JP-8、煤油，和醇类，包括甲醇和乙醇。
第二级管218环绕布置于第一级管208的周围。第二级管218具有第二级管入口220，用于接收氧和重烃燃料的混合物。第二级管218也具有第二级管出口222，用于导出第二级混合物的第二级反应转化产物。第二级管218可以具有第二级管218的统一直径长度，或者第二级管218可以呈锥形，例如在下部206处的直径较大，而上部204处的直径较小。第二级管出口222是用于将第二级混合物的第二级反应转化产物导入混合区216。
环绕在第二级管周围布置的是第三级管224。第三级管224具有第三级管入口226，其紧接混合区216，用于接收第一级混合物的第一级反应转化产物和第二级混合物的第二级反应转化产物的混合物。第三级管224具有第三级管出口228，用于从第三级管224导出第一级反应转化产物和第二级反应转化产物的混合物。第三级管224可以包括蒸汽转化催化剂225，用于进一步转化存在于混合物中的烃类。合适的蒸汽转化催化剂的例子包括与所述蒸汽转化催化剂214相同的催化剂。
螺旋管232延伸至大约第三级管224的长度。螺旋管232的第一端口234位于入口室233处。氧源242通过导管235经第一端口236连到入口室233，用于接收来自氧气区240的含氧气体。螺旋管232的第二端口247具有螺旋管出口244，用于将含氧气体导入第二级管218。合适的含氧气体的例子包括氧(O2)、空气等。
重燃料源241经重燃料管243与重燃料入口246相连。重燃料入口246连到紧接在第二端口247的螺旋管232上。合适的重燃料的例子包括汽油、煤油、JP-8、甲醇和乙醇。在另一实施方案中，相同的燃料源可用于重燃料(第一级烃燃料)和轻燃料(第二级烃燃料)。另外，如图2所示的分馏器，可以用于提供重燃料和轻燃料。在另一实施方案中，轻燃料和重燃料可以是相同的，并可来自同一来源。
反应器252环状地置于第三级管224的周围。反应器入口254能够把转化产物从第三级管出口228引入到反应器252。螺旋管232置于反应器252和第三级管224之间，来自第三级管224的气体经反应器252，从反应器入口254进入，经螺旋管232的周围，到达反应器出口256。气流分配区258使来自反应器出口256的气体进到催化转化区260。由第二个蒸汽入口257加入额外的蒸汽，用于为转化提供额外的冷却和转化所需的水。
催化转化区260环状地布置在反应器252的周围。催化转化区260包括催化剂262用于把转化产物进一步转化成氢气。合适的催化剂的例子包括三价铁的氧化物(Fe2O3)和三价铬的氧化物(Cr2O3)。其他类型的高温转化催化剂包括氧化铁和氧化铬，用下列物质助催化，如铜、铁的硅化物、载体上的铂、载体上的钯、和其他载体上的铂族金属，它们可单独或结合起来使用。催化剂可以是粉末状的，其高度基本上达到反应器252的高度。催化转化区260具有足够多的孔，以允许气体从气流分配区258通过并进入出口区268。在催化转化区260中的催化剂262由下部多孔板264和上部多孔板266固定装载。催化转化区260的产物气体从出口区268通过烃水蒸汽转化装置外壳出口270离开第三级转化装置200。
在本发明将烃类或醇类燃料转化成氢气和二氧化碳的第三个实施方案中，从轻燃料源217引入的燃料通过轻燃料管219到第一级管入口210。蒸汽从蒸汽源213引入，通过蒸汽管215至管入口210进入管208。轻燃料与蒸汽部分反应形成含有氢气和一氧化碳的第一级热转化产物物流。第一级热转化产物物流从第一级管208引入，通过第一级管出口212到混合区216。
一种例如空气的含氧气体从氧源242引入，通过导管235到入口室233，再到氧气区240进入螺旋管232第一端口入口236。把例如空气的含氧气体预热至约450℃的温度。在一优选的实施方案中，空气的流速大于约每秒40米。当含氧气体通过螺旋管232时，从重燃料源241由重燃料管243引入一种合适的重燃料蒸气。合适的重燃料例子包括JP-8、煤油和其他通常用于烃水蒸气转化的烃类燃料。也可以使用气体的烃，如甲烷和丙烷。含氧气体和重燃料的加入速率以使其足以在螺旋管232中混入，且在此混合物由第二级管入口220进入到第二级管218时，自发发生部分氧化反应形成含有蒸汽、一氧化碳和氧气的热的第二级转化产物物流为宜。在一种优选的实施方案中，含氧气体成切线通到第二级管218内部的四周。第二级混合物的烃类燃料部分反应形成含有氢气和一氧化碳的第二级热的转化产物物流。第二级管218中的热量可提供能量使第一级管208中的反应进行。
加入到第一级管208和第二级管218中的燃料在数量上可以相等，也可以不相等。第二级管218，即部分氧化室，例如可以在1375℃的温度下，燃料/氧气比约为2至1的比例下操作。从第二级管218到第一级管208的热传递可导致在第一级管208中发生部分水蒸汽转化，而温度会保持在约925℃。对于例如汽油和轻煤油这样的液体燃料，把较轻的燃料组分预汽化，以传递热量到第一级管208。重燃料在部分氧化区燃烧，这里的高温(约1375℃)能够以最小限度的碳化把燃料裂解。
来自第一级管208的第一级热的转化产物物流和来自第二级管218的第二级热的转化产物物流分别通过第一级管出口212和第二级管出口222，进入混合区216。分开的管允许在大约4或5比1这样高的燃料/氧之比下进行碳还原操作，由此减少烟灰的形成。其允许使用馏分燃料，如汽油或煤油，由此，重馏分类型的燃料优选引入到第二级管218中进行裂解大分子所需的高温燃烧，而轻馏分类型的蒸气引入到第一级管208中，与来自第二级管218的高温燃烧热接触而导致进行部分水蒸汽转化。第一级热的转化产物物流与第二级热的转化产物物流在混合区216混合。此混合物由混合区216经第三级管入口226，进入到第三级管224。
在第三级管224中，另一部分的燃料转化成氢气和一氧化碳形成第三级管转化产物物流。第三级管转化产物物流经由第三级管出口228排出。第三级管转化产物通过反应器入口254进入到反应器252，在此，转化产物物流从螺旋管232的周围通过，到反应器出口256。通过蒸气入口253可加入额外的蒸汽至反应器252中，用以提供额外的冷却和使转化产物物流中的烃类和一氧化碳进一步转化。转化产物物流从气流分配区258引入，通过催化转化区260，在此，转化产物物流通过催化转化区进一步把一氧化碳转化成氢气和二氧化碳，形成一氧化碳浓度约为0.5％(体积)的产物物流。产物物流经出口区268流出外壳出口270。
等效物
本领域的技术人员仅仅使用常规的实验方法将可认识到或可确定在此所述的本发明的许多具体的实施方案的等效物。这些等效物包括在权利要求书所要求的范围之内。

Claims (45)

1．一种用于将烃类燃料转化成氢气和二氧化碳的烃水蒸汽转化装置，其包括：
a)第一级反应器，其具有部分氧化反应区和分开的与所述的部分氧化反应区不同的蒸汽转化反应区，所述的第一级反应器在部分氧化反应区处具有第一级反应器入口，和在蒸汽转化区处具有第一级反应器出口；
b)螺旋管，其延伸在第一级反应器周围，所述的螺旋管具有用于连接氧源的第一端口，和连到第一级反应器入口的第二端口，在此，来自氧源的氧气通过所述的螺旋管导入至所述的第一级反应器；和
c)第二级反应器，其具有第二级反应器入口和第二级反应器出口，所述的第二级反应器环绕布置在第一级反应器周围，在此，所述的螺旋管布置在第一级反应器和第二级反应器之间，且来自第一级反应器的气体可被导入通过所述的第二级反应器。
2．权利要求1所述的烃水蒸汽转化装置，其中所述的第一级反应器入口成切线布置，以在第一级反应器内部的周围导入氧气。
3．权利要求1所述的烃水蒸汽转化装置，其中所述的氧源包括空气。
4．权利要求1所述烃水蒸汽转化装置，其中螺旋管连到烃源上，使氧气和烃能在螺旋管中混合。
5．权利要求4所述的烃水蒸汽转化装置，其中螺旋管连到蒸汽源上，使氧气和烃与来自蒸汽源的蒸汽在螺旋管内混合。
6．权利要求1所述的烃水蒸汽转化装置，其中所述的蒸汽转化区包括第一级催化剂。
7．权利要求6所述的烃水蒸汽转化装置，其中所述的第一级催化剂包括镍催化剂。
8．权利要求1所述的烃水蒸汽转化装置，其中所述的第一级反应器包括点火装置。
9．权利要求1所述的烃水蒸汽转化装置，其中第三级反应器环绕布置在第二级反应器周围，且所述的第三级反应器具有第三级反应器入口和第三级反应器出口，以通过第三级反应器从第二级反应器导出气体。
10．权利要求9所述的烃水蒸汽转化装置，其中所述的第三级反应器具有高温转化区。
11．权利要求10所述的烃水蒸汽转化装置，其中所述的高温转化区具有第二级催化剂。
12．权利要求11所述的烃水蒸汽转化装置，其中所述的高温转化区的第二级催化剂包括氧化铁。
13．权利要求12所述的烃水蒸汽转化装置，其中所述的第三级反应器具有低温转化区。
14．权利要求13所述的烃水蒸汽转化装置，其中所述的低温转化区具有第三级催化剂。
15．权利要求14所述的烃水蒸汽转化装置，其中所述的低温转化区的第三级催化剂包括铜。
16．一种用于将烃类燃料转化成氢气和二氧化碳的方法，其包括如下步骤：
a)通过螺旋管导入氧气，所述的螺旋管布置在第一级反应器的周围；
b)将烃蒸气和水蒸汽导入至螺旋管以形成氧气、烃蒸气和水蒸汽的混合物；
c)将氧气、烃蒸气和水蒸汽的混合物导入至第一级反应器，在此，所述的烃蒸气自发地部分氧化形成含有一氧化碳和氢气的热的转化产物物流；
d)将热的转化产物物流中的剩余烃蒸气进行水蒸汽转化以形成氢气和一氧化碳；
e)导入热的转化产物物流通过螺旋管，在此，热的转化产物物流加热螺旋管内的混合物；
f)通过高温转化反应将转化产物物流中的部分一氧化碳气体转化成二氧化碳；和
g)通过低温转化反应将转化产物物流中的至少一部分剩余的一氧化碳气体转化成二氧化碳，从而形成含有氢气和二氧化碳的产物物流。
17．权利要求16所述的方法，其中所述的氧气成切线地导入至第一级反应器内部的周围。
18．权利要求16所述的方法，其中所述的氧气包括空气。
19．权利要求16所述的方法，其中所述的烃蒸气和氧气在其进入第一级反应器之前混合。
20．权利要求19所述的方法，其中所述的烃蒸气和氧气与水蒸汽进一步混合。
21．权利要求16所述的方法，其中所述的烃蒸气在第一级催化剂存在下进行蒸汽转化。
22．权利要求22所述的方法，其中所述的第一级催化剂包括镍催化剂。
23．权利要求16所述的方法，其中所述的蒸汽转化在200℃至900℃温度范围之间进行。
24．权利要求16所述的方法，其中所述的高温转化反应在第二级催化剂存在下进行。
25．权利要求24所述的方法，其中所述的第二级催化剂包括氧化铁。
26．权利要求16所述的方法，其中所述的高温转化反应在300℃至600℃温度范围之间进行。
27．权利要求16所述的方法，其中所述的低温转化反应在第三级催化剂存在下进行。
28．权利要求27所述的方法，其中所述的第三级催化剂包括铜。
29．权利要求16所述的方法，其中所述的低温转化反应在约150℃至300℃温度范围之间进行。
30．一种用于将烃类燃料转化成氢气和二氧化碳的烃水蒸汽转化装置，其包括：
a)第一级管，其中所述的第一级管具有用于接收含氧气体和第一级燃料的第一级混合物的第一级管入口，和用于传导所述的第一级混合物的第一级反应转化产物的第一级管出口；
b)第二级管，其环绕布置在第一级管周围，其中所述的第二级管具有用于接收第二级燃料和水蒸汽的第二级混合物的第二级管入口，所述的第二级管具有用于导入所述的第二级混合物的第二级反应转化产物的第二级管出口；
c)催化转化区，其环绕布置在第二级管周围，其中所述的第一级反应转化产物和第二级反应转化产物可分别通过第一级管出口和第二级管出口导入至用于进一步转化所述混合物的催化转化区。
31．权利要求30所述的装置，其中烃类燃料分馏器连接在所述的第一级管入口和第二级管入口处，在此，所述的分馏器可从用于后续导入至部分氧化区的烃类燃料中分离出重组分，在此可以从用于后续导入至蒸汽转化区的烃类燃料中分离出轻组分。
32．权利要求30所述的烃水蒸汽转化装置，其中所述的氧气包括空气。
33．权利要求30所述的烃水蒸汽转化装置，其中所述的第一级燃料和第二级燃料是相同的。
34．权利要求30所述的烃水蒸汽转化装置，其中所述的第一级燃料包括馏出的燃料、汽油和醇类。
35．权利要求30所述的烃水蒸汽转化装置，其中所述的第二级燃料包括馏出的燃料、汽油和醇类。
36．权利要求30所述的烃水蒸汽转化装置，其中催化转化区的催化剂选自镍、钯、铂、铑和钌。
37．一种用于将烃类燃料转化成氢气和二氧化碳的方法，其包括如下步骤：
a)将含氧气体和第一级烃类燃料的第一级混合物导入至第一级管中，在此，所述的第一级混合物的第一级烃类燃料自发地部分氧化形成第一级热的含有氢气和一氧化碳的转化产物物流；
b)将第二级烃类燃料和水蒸汽的第二级混合物导入至环绕布置在所述第一级管周围的第二级管中，在此，所述的第二级混合物的第二级烃类燃料的部分水蒸汽转化形成含有氢气和二氧化碳的第二级热的转化产物物流；
c)将所述的第一级热的转化产物物流和第二级热的转化产物物流通过催化转化区以使所述的转化产物物流进一步转化。
38．权利要求37所述的方法，其中所述的烃类燃料在导入至第一级管和第二级管之前被分馏成烃类燃料的重组分和轻组分，所述的重组分后续导入至所述的部分氧化区，所述的轻组分导入至所述的蒸汽转化区。
39．权利要求37所述的方法，其中空气是氧气。
40．权利要求37所述的方法，其中所述的第一级混合物的第一级烃类燃料和第二级混合物的第二级烃类燃料是相同的。
41．权利要求37所述的方法，其中所述的催化转化区包括第一级催化剂。
42．权利要求41所述的方法，其中所述的第一级催化剂选自镍、钯、铂、铑和钌。
43．权利要求37所述的方法，其中所述的第一级混合物的第一级烃类燃料选自馏出的燃料、汽油、甲醇，乙醇、醇类和醚类。
44．权利要求37所述的方法，其中所述的第二级混合物的第二级烃类燃料选自馏出的燃料、汽油、甲醇，乙醇、醇类和醚类。
45．一种用于将包括第一级烃类燃料和第二级烃类燃料的烃类燃料转化成氢气和二氧化碳的烃水蒸汽转化装置，其包括：
a)第一级管，其中所述的第一级管具有用于接收水蒸汽和第二级燃料的第一级混合物的第一级管入口，和用于传导所述的第一级混合物的第一级反应转化产物的第一级管出口；
b)第二级管，其环绕布置在第一级管周围，其中所述的第二级管具有用于接收第一级燃料和含氧气体的第二级混合物的第二级管入口，所述的第二级管具有用于传导所述的第二级混合物的第二级反应转化产物的第二极管出口；
c)催化转化区，其环绕布置在第二级管周围，其中所述的第一级反应转化产物和第二级反应转化产物可分别通过第一级管出口和第二级管出口导入至用于进一步转化所述混合物的催化转化区。
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