CN101627106A - 在燃料处理应用中使用催化剂预燃烧器的方法 - Google Patents

在燃料处理应用中使用催化剂预燃烧器的方法 Download PDF

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CN101627106A
CN101627106A CN200780045925A CN200780045925A CN101627106A CN 101627106 A CN101627106 A CN 101627106A CN 200780045925 A CN200780045925 A CN 200780045925A CN 200780045925 A CN200780045925 A CN 200780045925A CN 101627106 A CN101627106 A CN 101627106A
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catalyst
fuel
gas
preburner
liquid fuel
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游立新
D·G·卡塞伊
K·H·源
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Texaco Development Corp
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Abstract

在燃料处理应用中在催化剂燃烧器上游使用催化剂预燃烧器例如阳极尾气氧化器(ATO)的方法。本方法制备可以在单个ATO中有效燃烧的含氢的气体混合物。催化剂预燃烧器将原料燃料转化为含氢的气体混合物。随后,该含氢的气体混合物在进入催化剂燃烧器前和需要的空气流、阳极尾气和变压吸附装置的废气混合。本方法致力于ATO的开车需求以及ATO能够在单个装置中燃烧液体和气体燃料的要求。

Description

在燃料处理应用中使用催化剂预燃烧器的方法
技术领域
本发明总体上涉及在燃料处理应用中在催化剂燃烧器上游使用催化剂预燃烧器(例如阳极尾气氧化器)的方法。
技术背景
燃料电池通过化学氧化-还原反应提供电能,并且与其它产生能量的形式相比,在清洁度和效率方面具有显著优势。通常,燃料电池使用氢气作为燃料,和将氧气作为氧化剂。产生的能量与反应物的消耗速率成正比。
缺少分布广泛的氢气基础设施是抑制燃料电池广泛使用的显著缺点。与目前大多数能源产生系统中使用的烃燃料相比,氢气具有相对低的体积能量密度,且更难于储存和运输。克服这个困难的一种方法是使用重整器将烃转化为可被用作燃料电池原料的富氢气体物流。
烃基燃料,例如天然气、LPG、汽油和柴油,需要转化过程以被用作大多数燃料电池的燃料来源。现有技术使用多步过程,其将最初的转化过程与数个过程组合。最初的过程最通常是蒸汽重整(SR),自热重整(ATR),催化部分氧化(CPOX),非催化部分氧化(POX)。净化过程通常由脱硫、高温水煤气变换、低温水煤气变换、选择性CO氧化或选择性CO甲烷化的组合组成。可供选择的过程包括氢选择性膜反应器和过滤器。
催化剂燃烧器,例如阳极尾气氧化器(ATO),对于燃料处理器和燃料电池的操作是必不可少的。单个的ATO必须能够有效燃烧燃料电池的废气和变压吸附装置的废气。此外,单个的ATO必须能够有效燃烧天然气、液态烃和醇。另外,单个的ATO必须具有液体燃料燃烧能力,以开车并补充燃料。虽然催化剂燃烧器,例如ATO,和传统的燃烧器相比具有优势,但存在与在燃料处理应用中操作ATO相关的问题。
与ATO的相关的一个问题包括难以使天然气催化剂燃烧器开车。具体地,天然气催化剂燃烧器开车需要大量的预热空气或者电力输入。在燃料处理应用中,天然气和/或空气必须被预热到高于天然气点火温度(约300℃)的温度,以在ATO中氧化。另外,为了控制催化剂床层的温度,需要很高的空气流量(氧碳比约为7),这对于1摩尔天然气需要约33.3摩尔空气。必须使用电加热器来保持催化剂床是热的,或必须使用大型换热器以便对天然气和/或空气进行预热。这些解决方案都存在一些设计和操作问题。
与ATO的相关的另一个问题包括要求在单个装置中燃烧液体和气体燃料。在燃料处理操作中,ATO必须能够在单个装置中燃烧各种燃料,包括液体和气体燃料。这样的要求提出了设计上的挑战。
本发明致力于ATO的开车需求以及ATO能够在单个装置中燃烧液体和气体燃料的要求。
发明内容
本发明提供在燃料处理应用中在催化剂燃烧器上游使用催化剂预燃烧器例如阳极尾气氧化器(ATO)的方法。本发明的方法制备可以在单个ATO中有效燃烧的含氢的气体混合物。催化剂预燃烧器将原料燃料转化为含氢的气体混合物。随后,该含氢的气体混合物在进入催化剂燃烧器前和需要的空气流混合。
当如本发明一样利用预燃烧器时,减少了天然气催化剂燃烧器的加热需求。首先,催化剂预燃烧器的加热需求远少于普通的催化剂燃烧器。其次,因为氢气可以在约40℃下点火,所以在随后的催化剂燃烧器中不需要加热空气。因此对于天然气燃料,明显减少了加热需求。
此外,当如本发明一样利用预燃烧器时,增大了天然气催化剂燃烧器的燃料转化率。在催化剂预燃烧器中,使用小于1的氧碳比导致了通过部分氧化而在气体混合物中存在一些氢气。因为氢气在随后的催化剂燃烧器中容易点火,所以总的燃料转化率将是高的。
另外,当如本发明一样利用预燃烧器时,不需要双燃料催化剂燃烧器。如果使用液体燃料混合物,则催化剂预燃烧器只需要具有液体氧化的能力。催化剂预燃烧器不需要燃烧气体,和随后的催化剂燃烧器不需要燃烧液体燃料-催化剂燃烧器只需要燃烧气体燃料。因而解决了对液体燃料的设计挑战。
最后,当如本发明一样利用预燃烧器时,提供另外的好处-从预燃烧器获得的氢气可以在第二反应区内与氧气混合,从而消除了反应区外爆炸性混合物的形成。
附图说明
参考所附附图提供说明,其中:
图1描述了燃料处理器的简单工艺流程图。
图2说明了一个紧凑式燃料处理器的实施方案。
图3说明了燃料处理应用的阳极尾气氧化器上游的催化剂预燃烧器的一个实施方案。
具体实施方式
阳极尾气氧化器(ATO)对燃油处理器和燃料电池的操作是必不可少的。本发明提供了在燃料处理应用中在ATO上游使用催化剂预燃烧器的方法。
一般来说,燃料处理器是将烃燃料转化为富氢气体的装置。在一个实施方案中,本文描述的紧凑式燃料处理器从烃燃料生产富氢气体物流,以用于燃料电池中。然而,预期本发明方法的其它可能应用,包括其中需要使用氢气物流的任何应用。因此,虽然本文描述的发明是与燃料电池联合使用,但是本发明的范围并不仅限于该应用。每个示例性实施方案描述了燃料处理器或者使用燃料处理器的过程,其中将烃燃料原料导引通过燃料处理器。
燃料处理器中使用的烃燃料在环境条件下可以是液体或气体,只要它可以气化。本文所用的术语“烃”包括能够从部分氧化或者蒸汽重整反应制备氢气的含有C-H键的有机化合物。不排除化合物的分子结构中存在碳和氢之外的原子。因此,适用于燃料处理器的燃料包括并不仅限于烃燃料例如天然气、甲烷、乙烷、丙烷、丁烷、石脑油、汽油、柴油燃料,和醇例如甲醇、乙醇、丙醇等。
燃料处理器原料包括烃燃料、氧气和水。氧气可以是空气、富氧空气、或基本纯氧的形式。水可以作为液体或者蒸气加入。原料组分的组成百分比通过如下所讨论的所需操作条件决定。
燃料处理器排出物物流包含氢气和二氧化碳,也可以包含一些水、未转化的烃、一氧化碳、杂质(如硫化氢和氨)和惰性组分(如氮气和氩气,特别是当空气是原料物流的组分时)。
参照图1,图1描述了燃料处理器的简单工艺流程图,说明了在将烃燃料转化为富氢气体中包括的过程步骤。本领域技术人员应理解,在通过本文公开的反应器的反应物的流动中,需要经过一定数量的渐进顺序。
过程步骤A是自热重整过程,其中两个反应,部分氧化(下文的式I)和任选的蒸汽重整(下文的式II)进行组合,以将原料物流F转化成含有氢气和一氧化碳的合成气。式I和式II是示例性的反应式,其中将甲烷看作烃:
CH4+1/2O2→2H2+CO    (I)
CH4+H2O→3H2+CO      (II)
部分氧化反应非常快速地发生,完全转化加入的氧气并产生热量。蒸汽重整反应发生得较慢并消耗热量。原料物流中较高的氧气浓度有利于部分氧化反应,而较高的水蒸气浓度有利于蒸汽重整。因而氧和烃的比以及水和烃的比成为特征参数。这些比影响了操作温度和氢气的产率。
自热重整步骤的操作温度范围可以在约550℃-约900℃,取决于进料的条件和催化剂。本发明使用包含或不包含蒸汽重整催化剂的部分氧化催化剂的催化剂床。催化剂可以是任何形式,包括粒料、球形、挤出物、整体料等。部分氧化催化剂应为本领域技术人员所熟知,和通常由整体料、挤出物、粒料或其它载体上的氧化铝洗涂层(washcoat)上的贵金属例如铂、钯、铑、和/或钌组成。已经使用过非贵金属,如镍或者钴。其它的洗涂层如氧化钛、氧化锆、氧化硅、氧化镁已经在文献中列举。多种附加材料例如镧、铈和钾已经在文献中列举作为改进部分氧化催化剂性能的“促进剂”。
蒸汽重整催化剂应为本领域技术人员所熟知,和可以包含镍和一定量的钴或贵金属例如铂、钯、铑、钌和/或铱。催化剂可以负载于例如氧化镁、氧化铝、氧化硅、氧化锆或铝酸镁中的一种或组合之上。可替代地,蒸汽重整催化剂可以包含镍,优选负载于由碱金属例如钾促进的氧化镁、氧化铝、氧化硅、氧化锆或铝酸镁中的一种或组合之上。
过程步骤B是冷却步骤,用于将来自过程步骤A的合成气物流冷却至约200℃-约600℃、优选约300℃-约500℃、更优选约375℃-约425℃的温度,以优化合成气流出物的温度用于下一步骤。该冷却可以用加热槽、加热管或换热器完成,取决于设计规格以及回收/循环气体物流的热含量的需求。步骤B的一种示例性实施方案是使用换热器,该换热器利用原料物流F作为循环通过换热器的冷却剂。换热器可以是本领域技术人员已知的任意合适结构,包括管壳式、板式、螺旋式等。作为其替代或补充,冷却步骤B可以通过注入另外的原料组分例如燃料、空气或水完成。水是优选的,因为当水气化为蒸汽时能够吸收大量的热量。添加的组分的量取决于需要的冷却程度,且容易由本领域技术人员确定。
过程步骤C是纯化步骤。烃物流主要杂质的一种是硫,其被自热重整步骤A转化为硫化氢。过程步骤C中使用的处理中心优选包含氧化锌和/或其它能够吸收并转化硫化氢的材料,和可以包含载体(例如整体料、挤出物、粒料等)。脱硫通过根据以下反应式III将硫化氢转化为水而完成:
H2S+ZnO→H2O+ZnS    (III)
其它的杂质例如氯化物也可以被除去。反应优选在约300℃-约500℃、更优选约375℃-约425℃的温度下进行。氧化锌在约25℃-约700℃的宽温度范围内是有效的硫化氢吸收剂,和通过适当选择操作温度而提供优化处理步骤顺序的良好灵活性。
流出物物流接下来可以被送入混合步骤D,其中任选将水加入到气体物流中。加入的水当它气化时降低了反应物物流的温度,并向过程步骤E的水煤气变换反应提供更多的水(下文讨论)。水蒸气和其它的流出物物流组分通过流经惰性材料的处理中心进行混合,所述惰性材料例如有效混合和/或辅助水的气化的陶瓷珠或者其它类似材料。可替代地,可以随原料加入任何附加的水,和混合步骤可以重新确定位置,以为下文讨论的CO氧化步骤G中的氧化剂气体提供更好的混合。
过程步骤E是水煤气变换反应,其根据式IV将一氧化碳转化为二氧化碳:
H2O+CO→H2+CO2        (IV)
这是重要的步骤,因为一氧化碳除去对人是剧毒之外,对燃料电池也是有毒的。一氧化碳的浓度优选应该降低至可以被燃料电池容忍的水平,通常低于50ppm。通常,根据使用的催化剂,水煤气变换反应可以在150℃-600℃的温度下发生。在这些条件下,气体物流中大多数的一氧化碳在这个步骤中被转化。
低温变换催化剂在约150℃-约300℃下操作,和包含例如氧化铜,或者负载在其它过渡金属氧化物如氧化锆上的铜,负载在过渡金属氧化物或耐火载体如氧化硅、氧化铝、氧化锆等上的锌,或者负载于合适的载体如氧化硅、氧化铝、氧化锆等上的贵金属例如铂、铼、钯、铑或金。
高温变换催化剂优选在约3000-约600℃的温度下操作,和可以包含过渡金属氧化物例如氧化铁或氧化铬,和任选包含促进剂如铜或铁suicide。高温变换催化剂也包含载带的贵金属,例如载带的铂、钯和/或其它铂族成员。
进行该步骤的处理中心可以含有如前文所述的高温变换催化剂或低温变换催化剂或高温变换催化剂和低温变换催化剂的组合的填充床。该过程应该在适合水煤气变换反应的任何温度下操作,根据使用催化剂的种类,优选在150℃-约400℃的温度下。任选地,可以在变换反应器的处理中心中放置冷却元件例如冷却盘管,用来降低催化剂填充床内的反应温度。较低的温度有利于一氧化碳转化为二氧化碳。此外,通过向高温和低温变换提供在高温和低温变换步骤之间的脱硫组件的单独步骤,可以在高和低变换转化之间进行纯化处理步骤C。
过程步骤F’是一个实施方案中通过换热器进行的冷却步骤。换热器可以是任何适合的构造,包括管壳式、板式、螺旋式等。可替换地,可以采用热管或者其它形式的散热装置。换热器的目标就是降低气体物流的温度,以生产温度优选为约90℃-约150℃的流出物。
在步骤F’中向过程加入氧气。加入的氧气被下文讨论的过程步骤G的反应所消耗。氧气可以是空气、富氧空气或基本纯氧形式。可以设计换热器以提供空气和富氢气体的混合。可替代地,过程步骤D的实施方案可以用于进行混合。
过程步骤G是氧化步骤,其中将流出物物流中几乎所有的剩余一氧化碳转化为二氧化碳。这个处理在用于氧化一氧化碳的催化剂的存在下进行,所述催化剂可以是任意形式,例如粒料、球形、整体料等形状。用于一氧化碳氧化的催化剂是已知的,和通常包含贵金属(如铂、钯)和/或过渡金属(如铁、钴、锰),和/或贵金属或过渡金属的化合物、尤其是氧化物。优选的氧化催化剂是氧化铝洗涂层上的铂。所述洗涂层可以涂布于整体料、挤出成型、粒料或其它载体上。可以加入另外的材料例如铈或镧,以改进性能。文献中已经列举了很多其它配方,一些实践者宣称来自铑或氧化铝催化剂的优良性能。文献中已经列举了钌、钯、金和其它材料可用于该应用。
在过程步骤G中发生两个反应:希望的一氧化碳氧化(式V)和不希望发生的氢气氧化(式VI),如下所示:
CO+1/2O2→CO2    (V)
H2+1/2O2→H2O    (VI)
在低温下有利于首选的一氧化碳氧化。因为两个反应都产生热量,所以任选包括冷却元件例如在过程中放置冷却盘管可能是有利的。过程的操作温度优选保持在约90℃-约150℃。过程步骤G优选将一氧化碳的浓度降低到50ppm,这对燃料电池中的应用是合适的浓度,但是本领域技术人员应理解,本发明可以适于制备具有较高和较低一氧化碳浓度的富氢产品。
离开燃料处理器的流出物是含有一氧化碳和可能存在的其它组分如水、惰性组分(如氮气、氩气)、剩余的烃等的富氢气体。产品气体可以用作燃料电池的原料或用于其中需要富氢原料物流的其它应用。任选地,可以将产品气体送至进一步的处理,如除去二氧化碳、水或其它组分。
燃料处理器100包含一系列用于进行如图1所述的一般性过程的工艺装置。如本领域技术人员容易明白的,意图是工艺装置可以以多种构造进行使用。此外,本文描述的燃料处理器适合于与燃料电池联合使用,使得将本文描述的燃料处理器的富氢产品气体作为原料物流直接供应至燃料电池。
参照图2,如图2说明一种紧凑式燃料处理器的实施方案。图2中所示的燃料处理器200与图1中图示和上文描述的过程相似。烃燃料原料物流F被引入燃料处理器中,和排出富氢产品气体P。燃料处理器200包括几个工艺装置,每个工艺装置进行单独的操作功能,通常它们的结构如图2所示。在这个示例性实施方案中,烃燃料F进入第一室,进入螺旋式换热器201,螺旋式换热器201用燃料电池尾气T(在ATO214进入燃料处理器200)预热原料F。因为燃料处理器中发生多个放热的反应,所以本领域技术人员应理解在这种应用中也可能存在数种其它的热联合机会。该经过预热的原料随后通过用于在反应器入口处实现接近完美的流动分布和低压降的同心扩散器进入脱硫反应器202。反应器202含有脱硫催化剂,和如图1的过程步骤C所述进行操作。(注意这个步骤和图1中提供的过程步骤顺序不一致。这是本领域技术人员为了处理多种烃燃料原料和/或制备更纯的产品而优化过程构造中可能实施的专利权范围内的最初实例。)来自反应器202的脱硫燃料随后通过同心扩散器收集并与空气A混合,混合物被导向换热器203。在该示例性实施方案中,换热器203是螺旋式换热器,其用燃料电池尾气T(在ATO214进入燃料处理器200)加热该混合的燃料/空气物流。
预热后的燃料/空气混合物进入到第二室,保持预热温度或者通过位于两个室之间的电线圈加热器204升高温度。预热后的燃料/空气混合物进入到螺旋式换热器205中,其用自热重整器(ATR)206流出物物流将物流预热至自热重整反应温度。预热的水(在换热器212处进入燃料处理器200)在进入换热器205之前和预热的燃料/空气物流混合。预热的燃料-空气-水混合物经过同心扩散器离开换热器205,然后被送入ATR206,这和图1中的过程步骤A相对应。扩散器甚至允许在ATR 206入口处的流动分布。来自ATR206的热氢产品经过同心扩散器收集,并返回换热器205进行热量回收。在这个实施方案中,换热器205被直接安装在ATR206的上部,以使流程最短,因而减少了能量的损失并改进了整个的能量效率。可以在弯管处插入流动调节叶轮,以实现通过ATR206的低压降和均匀流动。
来自换热器205的冷却的氢气产品随后通过同心扩散器导引至脱硫反应器207,这和图1中的过程步骤C相对应。脱硫后的产品然后被加入催化变换反应器208,这和图1中的过程步骤E相对应。提供冷却盘管209以控制放热变换反应的温度,这改进了一氧化碳的转化率,导致更高的效率。在该实施方案中,冷却盘管209还预热ATR206的进料,进一步提高了热量回收和燃料电池的效率。变换反应产品随后经过同心扩散器收集,和在螺旋式换热器210中冷却,其也预热了水进料W。
随后将空气A加入冷却的变换反应产物,然后其导向同心扩散器,加入优选的CO氧化反应器211。反应器211将痕量的一氧化碳氧化为二氧化碳,这与图1中的过程步骤G相对应。可以在弯管处插入流动调节叶轮,以实现通过反应器211的短流程和均匀低压降。流出的纯化氢气物流随后通过同心扩散器收集且进入到换热器212,换热器212将热能回收到水进料W中。冷却的氢气物流随后在分离器213中闪蒸以除去过量的水W。来自分离器213的氢气物流P之后适于氢气用户,如燃料电池。
在如图2中描述的实施方案中,将来自燃料电池的组合的阳极和阴极排出气体物流加入燃料处理器200中,以从燃料电池中没有转化的氢气中回收热量。燃料电池和燃料处理器的联合大大提高了从燃料电池发电的整体效率。燃料电池尾气T通过同心扩散器流入ATO214。氢气以及可能的甲烷和其它轻烃的滑流根据以下反应被催化氧化:
CH4+2O2→CO2+2H2O    (VII)
H2+1/2O2→H2O        (VIII)
反应式VII和VIII在ATO214中发生,ATO214可以是固定床反应器,由珠状催化剂粒料、或者优选的整体料结构的催化剂组成。热反应器流出物通过同心扩散器收集和导入换热器203中,以用来自反应器202的燃料/空气混合物回收热量。随后,在分离器215中闪蒸之前,在换热器201中进一步回收燃料电池尾气物流T的热量。分离出的水连接至处理器流出物水物流W,和排出的气体随后排放至大气。
参照图3,图3说明了燃料处理应用中使用的催化剂预燃烧器301的一个实施方案。催化剂预燃烧器301位于催化剂燃烧器303的上游。混合器302位于催化剂预燃烧器301的下游,催化剂燃烧器303的上游。在优选实施方案中,催化剂燃烧器303是ATO。气体燃料混合物304与第一空气流305一起被加入催化剂预燃烧器301中。催化剂预燃烧器301产生催化剂预燃烧器排出气体306,其与第二空气流307一起被加入混合器302。此外,来自燃料电池的阳极尾气或来自变压吸附装置309的废气也可以被加入混合器302中。仅将补充燃料(天然气或液体燃料)和第一空气加入预燃烧器。第二空气、预燃烧器排出气体、阳极尾气或来自变压吸附装置的废气可以被加入混合器。
加入催化剂预燃烧器301的气体燃料混合物304可以是燃料例如天然气;但是也可能包含其它气体燃料,例如丁烷、丙烷等。当使用天然气时,氧碳比需要是为0-1,优选为0.3-0.7(对应于空气流量为每摩尔天然气0-4.8摩尔空气)。优选的例子是氧碳比为0.5(每摩尔天然气2.4摩尔空气)。在不使用催化剂预燃烧器301的条件下,将要求氧碳比为7(每摩尔天然气33.3摩尔空气)。该第一空气流305更容易加热,因为其流量小很多(与33.3相比仅为2.4),和/或催化剂预燃烧器301的床层温度更容易保持是热的。此外,催化剂预燃烧器301的空速小于ATO 303,这导致好的燃料转化率。另外,当进入催化燃烧器303的总流量较少时,气体和床层之间的换热也减少,且也更容易保持催化剂燃烧器303的催化剂床层是热的。
在以上说明中,图3,当气体燃料混合物304进入催化剂预燃烧器301时,可以使用液体燃料例如液化石油气(LPG)、汽油、柴油、喷气燃料、甲醇、乙醇等以代替天然气。当使用液体燃料时,将需要液体燃料气化器。
催化剂预燃烧器301可以是粒料填充或整体料。可以使用部分氧化催化剂例如铂(Pt)、钯(Pd)、钌(Ru)。
下表提供物流的摩尔分数、流量和温度的Aspen
Figure G2007800459256D00101
模拟的结果。
  催化剂预燃烧器的排出气体   混合器的排出气体  ATO的排出气体
  CH4   3.07   0.37   0.00
  O2   0.00   18.45   14.98
  N2   40.89   74.38   76.85
  H2   35.62   4.32   0.00
  CO   17.37   2.11   0.00
  CO2   1.31   0.16   2.72
  H2O   1.74   0.21   5.45
  总流量(kmol/hr)   4.60   37.93   36.71
  温度(℃)   711.1   118.2   745.4
尽管已经根据优选或示例性实施方案中描述了本发明的方法,但是本领域技术人员将显而易见可以在不偏离本发明的概念和范围的条件下对本文描述的方法进行改变。为本领域技术人员显而易见的所有这些类似替代和修改视为在所附权利要求中陈述的本发明的范围和概念内。

Claims (17)

1、一种在燃料处理应用中使用催化剂预燃烧器的方法,该方法包括:
在催化剂燃烧器的上游提供所述催化剂预燃烧器,其中所述催化剂预燃烧器产生催化剂预燃烧器的排出气体;
在所述催化剂预燃烧器的下游和所述催化剂燃烧器的上游之间提供混合器,其中所述混合器产生混合器的排出气体;
将带有一次空气流的气体混合物加入所述催化剂预燃烧器;
将带有二次空气流的所述催化剂预燃烧器的排出气体加入所述混合器;和
将所述混合器的排出气体加入所述催化剂燃烧器。
2、根据权利要求1所述的方法,其中所述催化剂燃烧器是阳极尾气氧化器。
3、根据权利要求1所述的方法,其中所述催化剂预燃烧器、所述混合器和所述催化剂燃烧器整化成单个装置。
4、根据权利要求3所述的方法,其中所述单个装置是圆柱形的罐子。
5、根据权利要求1所述的方法,其中所述气体混合物包含天然气。
6、根据权利要求5所述的方法,其中所述催化剂预燃烧器的氧碳比是在0和1之间。
7、根据权利要求6所述的方法,其中所述的氧碳比是0.5。
8、根据权利要求5所述的方法,其中所述一次空气流为每1摩尔所述天然气在0和4.8摩尔之间。
9、根据权利要求8所述的方法,其中所述一次空气流为每1摩尔所述天然气2.4摩尔。
10、根据权利要求1所述的方法,其中所述气体混合物包含丙烷。
11、根据权利要求1所述的方法,其中所述气体混合物包含液体燃料。
12、根据权利要求11所述的方法,其中所述液体燃料是液化石油气。
13、根据权利要求11所述的方法,其中所述液体燃料是汽油。
14、根据权利要求11所述的方法,其中所述液体燃料是柴油。
15、根据权利要求11所述的方法,其中所述液体燃料是喷气燃料。
16、根据权利要求11所述的方法,其中所述液体燃料是甲醇。
17、根据权利要求11所述的方法,其中所述液体燃料是乙醇。
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