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CN100574866C - 催化反应器 - Google Patents

催化反应器 Download PDF

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CN100574866C
CN100574866C CN200680008498A CN200680008498A CN100574866C CN 100574866 C CN100574866 C CN 100574866C CN 200680008498 A CN200680008498 A CN 200680008498A CN 200680008498 A CN200680008498 A CN 200680008498A CN 100574866 C CN100574866 C CN 100574866C
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reactor
reaction
pressure
fischer
pressure vessel
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CN101142017A (zh
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M·J·鲍
J·维图奇
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GTL Microsystems AG
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GTL Microsystems AG
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Abstract

用于Fischer-Tropsch合成的紧凑型催化反应器(50)，包括反应模块(70)，该反应模块限定了交替设置的多个第一和第二流动通道，分别用于运送气体混合物和冷却剂。在每个发生合成反应的流动通道中提供可去除的气体可渗透催化剂结构(82)，该催化剂结构具有基底，例如金属薄片。反应模块(70)被装在压力容器(90)中，压力容器中的压力被设定成基本与高压反应气体混合物的压力基本相等。因此模块中的所有流动通道处于周围环境的压力下或处于压缩中，任何部分都没有处在拉伸中。这简化了模块的设计，并且提高了能够被催化剂占有的反应体积的比例。

Description

催化反应器
本发明涉及一种催化反应器，该反应器适用于将天然气转化为长链烃的化学方法中，尤其适用于进行Fischer-Tropsch合成，本发明还涉及包括这种执行所述化学方法的催化反应器的装置。
在WO 01/51194和WO 03/048034(Accentus plc)中描述了一种方法，在该方法中甲烷与蒸汽在第一催化反应器中反应生成一氧化碳和氢；产生的气体混合物随后用于在第二催化反应器中进行Fischer-Tropsch合成。结果是将甲烷转化成更高分子量的烃，这些烃在环境条件下通常为液体。该方法的两个阶段，即蒸汽/甲烷重整和Fischer-Tropsch合成分别需要不同的催化剂和向反应气体传递或来自反应气体的热，因为反应分别吸热和放热。两个不同阶段的反应器必须符合某些不同的需要：与蒸汽/甲烷重整相比，Fischer-Tropsch合成通常在较高压力和较温度下进行；在Fischer-Tropsch反应器的热传导通道中仅仅需要一种冷却剂流体，而蒸汽/甲烷重整需要的热通常通过催化燃烧提供，因此需要合适的催化剂。
在每种情况中反应器优选为堆叠的板形式，具有在板之间界定的流动通道，不同流体的流动通道在叠层中互相交互。在那些需要催化剂的通道中，优选为波纹结构的金属基底，在基底的难熔金属涂层中负载催化剂，当催化剂失效后能够将这种波纹结构从通道中除去。然而，两种流体之间压差很大时，将趋向导致板弯曲，使得在催化剂结构和板之间的热传递受阻，并且可能很难除去或替换催化剂结构；而且如果板必须足够坚固以抵抗压差，则板必须更加厚和/或通道更窄，并且作为反应器总体积的一部分的流动体积将趋向减少。
根据本发明，提供了一种用于Fischer-Tropsch合成的紧凑型催化反应器，包括反应模块，所述模块限定了多个在模块中交替设置的第一和第二流动通道，分别用于运送第一和第二流体，第一流体为进行Fischer-Tropsch合成的气体混合物，其压力高于环境压力，第二流体为冷却剂流体，其中每个发生化学反应的流动通道中都含有可去除的气体可渗透催化剂结构，该催化剂结构结合在金属基底上，其中反应模块装在压力容器中，将该压力容器内的压力设定为基本上等于任何较高压力流体的压力。
因为压力容器中的压力基本上为较高压力流体的压力，所以叠层板(the stack of plates)内的所有流动通道都处在环境压力下或处在加压下。因此叠层板的任何部分都没有处在拉伸状态。优选气体混合物为较高压力的流体，并且该气体混合物被设置成流过至少部分压力容器，以到达第一流动通道或(在已进行完Fischer-Tropsch合成后)离开第一流动通道。已完成Fischer-Tropsch合成后的气体混合物随后流过压力容器的一个优点是压力容器能够提供产物烃液滴和气体产物之间的第一级分离。
因此，在第二方面，本发明提供了用于Fischer-Tropsch合成的紧凑型催化反应器，包括密封在压力容器中合适的反应模块，其中压力容器内的压力被设定为基本上等于Fischer-Tropsch反应通道内的压力。
Fischer-Tropsch反应通常在大约200℃的温度下进行，所以可以选择很宽范围的材料来制备反应器模块。例如反应器模块可以由铝合金、不锈钢或高镍合金或其它铁合金制备。
优选催化剂结构的金属基底为铁合金，当被加热时所述铁合金形成了附着的氧化铝表面涂层，例如含有铝(aluminium-bearing)的低合金钢，例如具有15％铬、4％铝和0.3％钇的铁(即铁合金(Fecralloy)(TM))。当在空气中加热这种金属时，其形成了一种附着的铝氧化物涂层，该涂层保护合金不会受到进一步的氧化和腐蚀。在难熔金属覆层为铝覆层的地方，该覆层与表面上的氧化物涂层结合。基底可以是金属丝网或毡片，但是优选的基底是薄金属薄片，例如厚度小于100μm的薄片，并且基底可以是波纹状、凹陷状或皱褶状。
这种与催化材料结合的催化剂结构可以嵌入流动通道中，用于Fischer-Tropsch反应的流动通道与流动通道互相交替以除去热量。流动通道内的催化剂结构的金属基底增加了热传递和催化剂表面积。催化剂结构可以从模块中的通道中移出，因此如果催化剂失效可以被替换。
催化剂模块可以包括叠层板，例如每个板中的凹槽可以限定第一和第二流动通道，所述板堆叠在一起随后结合在一起。可选择地，流动通道可以通过薄金属薄片界定，这些薄金属薄片为齿形并且与平板相互堆叠；流动通道的边沿可以通过密封条界定。例如通过扩散粘结、钎焊或热等静压将形成反应模块的叠层板结合在一起。本发明的一个特殊的优点为结构材料(不包括催化剂)组成的反应模块的体积比例可以小于60％，优选小于50％，甚至可以小于35％。
因此用于处理天然气以获得长链烃的装置可以结合甲烷与蒸汽反应生成合成气的蒸汽/甲烷重整反应器和本发明的生成长链烃的Fischer-Tropsch反应器结合。为了确保必需的良好热接触，Fischer-Tropsch反应通道优选小于10mm深度。
仅通过实施例对本发明作进一步更详细的描述，关于附图，其中：
图1显示了结合本发明反应器的化学装置的流程图。
图2显示了适用于Fischer-Tropsch合成的反应模块的部分截面图。
图3显示了结合有图2的反应模块的反应器的截面图。
本发明涉及将天然气(主要为甲烷)转化为长链烃的化学方法。该方法的第一阶段包括蒸汽重整，即反应类型：
H2O+CH4→CO+3H2
该反应吸热，并且可以通过第一气体流动通道中的铑或铂/铑催化剂催化。可以通过易燃气体例如甲烷或氢的燃烧来提供该反应需要的热量，其中易燃气体的燃烧放热并且可以被临近的第二气体流动通道中的钯催化剂催化。在两种情况中催化剂优选承载在稳定的氧化铝载体上，其中氧化铝载体通常在金属基底上形成了小于100μm厚度的涂层。燃烧反应可以在大气压力下发生，而重整反应可以在4-5大气压下发生。燃烧产生的热将会通过将相邻通道分开的金属薄片传导。
随后使用蒸汽/甲烷重整产生的气体混合物进行Fischer-Tropsch合成以生成长链烃，即：
nCO+2nH2→(CH2)n+n H2O
该反应为放热反应，在高温(通常在190℃-280℃之间)和高压(通常在1.8MPa-2.1Mpa(绝对压力)之间)下、在催化剂例如铁、钴或熔凝磁铁存在下发生。用于Fischer-Tropsch合成优选的催化剂包括比表面积为140-230m2/g的γ-氧化铝涂层，具有大约10-40％的钴(按与氧化铝相对的重量记)、和小于10％钴重量的助催化剂(例如钌、铂或钆)、和碱性助催化剂例如氧化镧。
参考图1，以流程图的方式显示了总的化学方法，在该流程图中显示了装置组成部分。在该实施例中天然气进料5主要由甲烷与一定百分比的C2-C11高碳烃组成。通常这些高碳烃存在的量不超过10％v/v，这取决于天然气的来源。气体进料5例如可以为1.0Mpa(10个大气压)的压力。
通过阀门8将气体压力调整到0.6Mpa，随后在热交换器10中使用来自催化燃烧的热废气将气体5预热到约400℃，随后将气体5引入固体床脱硫系统12中。脱硫后的天然气5随后与蒸汽混合，例如在流体涡流混合器14中混合。在热交换器16中使用来自催化燃烧的热废气加热气体/蒸汽混合物，使得气体混合物的温度为500℃。混合物进入绝热固定床预重整器18，在那里与基于镍或铂/铑的甲烷化催化剂接触。高碳烃与蒸汽反应以形成甲烷和CO。
气体通常在450℃的较低温度下离开预重整器18，然后在进入重整器20之间通过阀19将压力降低到0.45Mpa(绝压)。重整器20为上述类型的紧凑型催化反应器。其由叠层板制备，所述板限定了吸热和放热反应的流动通道，具有良好的热接触，并且在通道中含有适当的催化剂。在重整反应器20中的重整通道含有重整催化剂，并且蒸汽和甲烷反应生成一氧化碳和氢。重整器中的温度从入口的450℃升高到出口时的大约800℃-850℃。向混合器14中供应的蒸汽和气体的流速使得进料到重整器20中的蒸汽和碳摩尔比在1.2-1.6之间，优选位于1.3-1.5之间。取决于气体5的高碳烃的含量，因此预重整器18入口处的蒸汽和碳的必须比这个以上值高。
通过短链烃和氢的混合物的催化燃烧来提供重整反应器20中的吸热反应的热。其中所述气体混合物为来自Fischer-Tropsch合成的尾气22；该尾气22与通过空气送风机24提供的空气流混合。在重整反应器20内的相邻流动通道内的燃烧催化剂上发生燃烧。燃烧气体通道与重整气体通道并流。
高于800℃的一氧化碳和氢的混合物从重整器20中流出，并且将该混合物通过流过蒸汽加热热交换器26，温度骤降到低于400℃。通过泵28该热交换器26提供水，因此用于重整过程的蒸汽通过控制阀30提供到混合器14中。气体混合物进一步在热交换器32中被冷却水冷却到大约60℃，使得过量的水冷凝并在通过旋风分离器33和分离容器34时得到分离。随后通过压缩机36将气体混合物压缩到大约2.5倍的压力，随后在通过第二旋风分离器41和分离容器42以除去任何冷凝的水之前再次被热交换器40冷却。分离的水再次循环回到蒸汽产生回路。随后在第二压缩机44中将气体压缩到20个大气压(2.0Mpa)。
高压一氧化碳和氢蒸汽随后进料到催化Fischer-Tropsch反应器50中，该反应器也是如上所述的由叠层板形成的紧凑型催化反应器，反应混合物流过一组通道，而冷却剂流过另一组通道。
来自Fischer-Tropsch合成的反应产物(主要为水和例如石蜡的烃)通过流过热交换器54来得到冷却以冷凝液体，流过旋风分离器56之后进入分离室58中，在该分离室中三相水、烃和尾气分离，并且烃产物在大气压下很稳定。在气相和过量氢气(Fischer-Tropsch尾气22)中残留的烃被收集和分离。一部分流过减压阀60以向重整器20(如上所述)中的催化燃烧过程提供燃料。残留的尾气62进料到驱动发电机64的燃气涡轮63中。
燃气涡轮64产生了装置需要的电力并且具有输出过剩电力的能力。需要电力的主要装置是压缩机36和44、泵24和28；电力还可以用来运行真空蒸馏单元，用于使工艺水产生蒸汽。
参考图2，显示了适用Fischer-Tropsch反应器50中的反应模块70，其中清楚的显示了该反应模块70的截面和各自部件。反应模块70由堆叠的厚度为1mm的板72组成，所述板彼此间隔以限定冷却流体的通道，该通道与Fischer-Tropsch合成通道相互交替。冷却流动通道由0.75mm厚度的齿形板74限定。在该实施例中齿的高度(通常在1-4mm之间)为2mm，并且沿边缘提供2mm厚的固体边缘衬条76，连续的连接带相隔6mm(以下将详细描述这种设置)。Fischer-Tropsch合成的通道高度为5mm，被方形截面的栅条78界定，其中栅条78高为5mm，彼此相隔350mm，并且垂直限定通过通道。
参考图3，显示了反应器50的截面，图中具有部分断开的反应模块70。如上提到的，反应模块70由平板72的叠层(stack)组成，所述平板彼此隔开以限定流动通道。叠层中互相交替的通道通常相互垂直定向。每个平板72为1.0mm厚和1070mm2。Fischer-Tropsch反应的通道含有承载催化剂的波纹状金属薄片82，并且通道从头部83直线延伸穿过反应模块70(如图所示从顶部延伸到底部)，其中高压合成气混合物通过管子84供应到所述头部83中；平板72通过横截面5mm2的栅条78支撑分开，其中栅条78从底部延伸到顶部并且间隔350mm，所以在连续的平板72之间具有3个并行的通道。对于冷却剂通道，平板72被齿形板74支撑隔开。冷却剂通道由0.25mm厚的薄片长条构成，沿薄片长条的长度形成了6mm宽度和2mm高的齿。齿状长条被剪切成段86并且这些段并行设置以限定横流通道(如图所示的水平方向)，以在入口端口87和出口端口88之间提供通道。靠近端口87和88的齿形长条86的末端被剪切成方形，其它末端被剪切成45°，设置齿状条的三角形片89以提供齿状条之间的连接。因此冷却剂的总的流动通道(如箭头所示)为Z字形通道，其部分与Fischer-Tropsch通道中的流动并流。平板72、栅条78和齿状长条86和89可以为铝合金，例如3003级(含有约1.2％锰和0.1％铜的铝)。
将叠层如上所述组合，然后例如通过钎焊结合在一起以形成反应模块70。皱褶状金属薄片催化剂载体82结合合适的催化剂，随后嵌入到Fischer-Tropsch合成的通道中。
图3中的箭头表示反应模块70使得冷却剂在经过入口87和出口88之间时3次通过Fischer-Tropsch通道的宽度，可替代地冷却剂可以正好2次通过通道的宽度，或也可以通过3次以上。冷却剂通道中相邻间隔的齿提供了抗弯曲的硬度。
反应模块70安装在碳钢压力容器90中，由支撑栅条92支撑。可以涂覆压力容器90的内表面，例如使用铬涂覆，以抗腐蚀或防止形成羰基铁。压力容器90可以是具有半球状末端的圆柱状。合成气的管道84、和向端口87和88提供或从以上端口提供冷却剂的管道97和98延伸通过压力容器90的壁。在容器90的底部具有一个液体产物的出口端口96，在容器90的顶部具有气体产物的出口端口100。
在反应器50的使用中，可以在0.7MPa下提供冷却剂，而在2.0MPa压力下提供合成气。Fischer-Tropsch合成的产物和未反应的气体从反应模块70的底部进入到压力容器90中，所以压力容器90中的压力也为约2.0MPa。来自反应模块的气体蒸汽中携带的液滴在速度下降时从大部分气流中分离出并滴落到底部，液滴可能改为撞击压力容器90中的表面并与之结合，使得液体向下流到底部并流出出口端口96。残留的气体通过出口端口100排出并被如图1所述处理。
为了增加以上提到的液/气分离机械装置，还可以在压力容器90中提供除雾填料。可选地或另外在压力容器90中安装旋风分离器，所述旋风分离器具有切线入口(气体蒸汽(可能含有液滴)通过该入口进入)、与出口端口100相连的气体出口、和除去的液滴的液体出口，该液体出口优选通过一个管子连接到低于容器90底部的液体产物的平面。
应当认识到外部压力容器壳90的使用有助于降低对向反应模块70提供强度的金属的需求，因为反应模块任何部分都不需要抗张力。冷却剂通道处在压力之下，但是齿状条74提供足够的硬度。因此压力容器壳90使得每单位体积能够具有更高负载的催化剂。这是因为例如72的板可以明显更薄，使得流动通道占有更大比例的反应模块体积，从而增加了空隙度，使得总催化剂保存量可以得到提高。例如在该Fischer-Tropsch反应器中，由结构材料组成的体积比例可以从超过70％降低到小于35％。这还最小化了流动通道的壁的弯矩，从而降低了变形，因此提高了催化剂金属薄片82与相邻壁之间的接触，从而提高了热传递，并且还使得拆除和安装更容易。应到意识到压力容器壳90具有相当简单的几何图形，所以其可以按现有压力容器规则设计。在发生反应模块70泄漏的情况下，压力容器壳还固有地提供一个二次容积，其形状容易隔离，并且容易运输和安装，而反应器总的尺寸并没有明显增加。
在图3中显示的Fischer-Tropsch反应器50的情况中，具有优点：反应模块70和壳90之间的空间可以被用来对气态和液态反应产物进行初始相分离，因此降低了后续产物分离器的体积和费用。还具有另一益处：可以使用相对廉价的材料例如铝来形成反应模块70。另一优点是因为在反应模块70的较低端(如图所示)没有提供顶盖，所以一旦压力容器90已经打开，催化剂金属薄片82就很容易被替换。

Claims (11)

1、一种用于Fischer-Tropsch合成的紧凑型催化反应器，包括反应模块，该反应模块限定了在模块中交替设置的多个第一和第二流动通道，分别用于运送第一和第二流体，第一流体为进行Fischer-Tropsch合成的气体混合物，并且其压力高于环境压力，第二流体为冷却剂流体；
其中每个发生化学反应的流动通道从反应模块的顶部直线延伸到其底部，并且通道中含有可去除的气体可渗透的催化剂结构，该催化剂结构结合了金属基底和用于Fischer-Tropsch合成反应的催化剂；
其中反应模块被装入压力容器中，压力容器内的压力被设定为基本上等于Fischer-Tropsch合成反应通道内的压力。
2、根据权利要求1所述的反应器，其中使气体混合物流过至少部分压力容器，以到达合成反应的流动通道或离开合成反应的流动通道。
3、根据权利要求2所述的反应器，其中经过合成反应的气体混合物随后流过压力容器，从而压力容器提供了液滴和气体产物之间的第一级分离。
4、前述任一权利要求的反应器，其中压力容器壳与反应模块的材料不同。
5、权利要求1-3任何之一的反应器，其中所述反应模块包括限定第一和第二流动通道的结构材料，并且由所述结构材料组成的反应模块体积比例小于60％。
6、根据权利要求5所述的反应器，其中所述比例小于50％。
7、根据权利要求1-3任何之一的反应器，其中每个进行合成反应的流动通道由平板限定，所述平板由栅条间隔支撑。
8、权利要求7所述反应器，其中栅条将平板隔开5mm。
9、权利要求1-3任何之一的反应器，其中每个冷却剂流体的流动通道由板限定，所述板由成型薄片间隔支撑。
10、根据权利要求1-3任何之一的反应器，其中限定第一和第二流动通道的部件包括铝合金。
11、用于将天然气转化为长链烃的装置，结合有用于产生合成气的蒸汽重整反应器、和用于生成长链烃的前述任一项权利要求所述的Fischer-Tropsch反应器。
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