CN1980732A - 紧凑型蒸汽重整装置 - Google Patents

紧凑型蒸汽重整装置 Download PDF

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CN1980732A
CN1980732A CNA2005800071843A CN200580007184A CN1980732A CN 1980732 A CN1980732 A CN 1980732A CN A2005800071843 A CNA2005800071843 A CN A2005800071843A CN 200580007184 A CN200580007184 A CN 200580007184A CN 1980732 A CN1980732 A CN 1980732A
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J·A·温宁
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Abstract

一种新型紧凑型蒸汽重整装置(1)在一个装置中结合了对天然气或其它燃料进行蒸汽重整，包括对CO进行后续清洗。通过在后续反应器(37，39，39a)中仔细地进行温度控制而对CO进行受控的催化清洗。借助蒸发器(24)受到压力控制的工作而有可能实施温度控制。

Description

紧凑型蒸汽重整装置
本发明涉及一种紧凑型蒸汽重整装置和一种进行蒸汽重整的方法。
与自热重整不同，在对烃进行蒸汽重整生成氢的过程中，用于生成气体的物料流和用于进行加热的物料流保持分开。按照这种方式，就避免了在进行蒸汽重整的过程中燃烧空气中的氮对氢产生稀释。
从DE 101 19 083 A1中已公知一种紧凑型蒸汽重整装置，其中工艺用水借助待冷却的重整产物基本上蒸发掉了。燃烧废热通过使空气预热而得到回收。通过采用无焰氧化工艺避免形成NOx。该重整装置允许进行快速输出调节并且具有高达大约80％的效率。
从WO 02/085781中已公知一种相似的在外部绝缘方面得到最优化的重整装置。
这些重整装置满足旨在预期。然而，需要在简化工艺调整和热回收效率等方面作出进一步的改进。此外，必须从重整产物中尽可能多地除去加入的CO。这一步骤必须进行得十分完全，从而使得在下游连接的对CO敏感的燃料电池不会被损坏。
从EP 1 031 374 A2中已公知将含有CO的工艺气体放入同时还被用作重整产物冷却器的所谓的CO氧化器中。通过使蒸发器中的流入的工艺气体蒸发，从而进行冷却。
基于前文所述，本发明的目的在于在工艺执行和热回收效率等方面对本文开始部分所述的紧凑型蒸汽重整装置作出改进。
本发明的目的借助如权利要求1所述的紧凑型蒸汽重整装置和采用如权利要求15所述的方法而得以实现。
根据本发明的紧凑型蒸汽重整装置包括一个通过燃烧器而被加热的反应器。具有较高热回收效率的预热装置被配置给所述燃烧器。这样就提高了重整工艺的效率。此外，所述重整装置包括一个后续反应器，所述后续反应器被设计用以执行转化反应、后续的氧化和/或由含在原始重整产物中的一氧化碳部分生成甲烷。所述后续反应器与保持后续反应器的温度以受控方式处于一固定水平的管式蒸发器热交换连接在一起。由此，即便是在负载变化的情况下，也可以保持后续反应的所需选择性。管式蒸发器致使在后续反应器中相对于时间和空间后期温度失控。在管式蒸发器中物料的流动致使在后续反应器中进行热传输，从而使得后续反应器能够快速适应负载变化。如果管式蒸发器和后续反应器以并流的方式进行工作，那么这是特别适用的。
通过确定蒸发器的温度，后续反应器的温度同时被固定在这些较窄的限值内，从而使得CO含量能够降至小于50ppm的数值。因此，工艺气体的后续催化处理、过滤或其它后续处理就成为多余的了。由紧凑型蒸汽重整装置产生的气体可被直接传导到氢燃料电池。
可以最简单的方式通过调节蒸汽压力从而能够设定后续反应器的温度。所有工作状态下的蒸汽生成温度与蒸汽压力一起被固定住。因此，在后续反应器与受压力调节的蒸发器之间的紧密的热连接，例如通过管式蒸发器作为盘管且可能存在的催化剂被布置在所述管道之间的空间中的实施例，形成了产生CO含量较低的氢的有利条件。
所述紧凑型蒸汽重整装置可包括连接到管式蒸发器或其它蒸发器上的喷射泵，所述各式蒸发器产生具有预先选定组分的燃料-流的混合物并且供应所述反应器。这样就借助一些控制技术为特别简单地控制所述紧凑型蒸汽重整装置提供了基础。例如，蒸汽量受到适当计量的给水量的控制。供应到重整装置的用于进行重整反应的燃料量不需要分开进行控制，而是通过喷射泵进行计量。
从附图、说明书或权利要求书中可以获得有利实施方式的其他细节。
附图中示出了本发明的典型实施例，其中：
图1示出了带有一个附接在其上的燃料电池的紧凑型蒸汽重整装置的示意图；
图2以图表的形式示出了工艺气体的温度曲线图；
图3以图表的形式示出了加热气体的温度曲线图；和
图4示出了紧凑型蒸汽重整装置的纵剖视图，其工作区域的布置与图2和图3中示出的曲线图相对应。
图1示出了蒸汽重整装置1的纵剖视图。该蒸汽重整装置1具有长度为L和直径为D的圆形横截面的外壳2。该蒸汽重整装置可以是圆柱形的，或者也可以是多个柱体组合在一起呈阶梯状。所有连接装置3优选传导通过其上端4。
接近底部的重整装置管道5被同心地布置在外壳2内并且距外壳2一定距离。被设置在外壳2与重整装置管道5之间的环形空间中填充有用于进行热绝缘的绝缘材料6。燃料和蒸汽混合物的供给管线7从上端4引出，开始先直线延伸，然后向下通过几个弯通过绝缘材料6到达位于重整装置管道下端的供给连接装置8。供给连接装置的下部呈杯状的端部构成用于进行实际重整工艺的反应器9的外壳。朝向内部，反应器9由内部重整装置管道11所界定，所述内部重整装置管道在底部呈杯状封闭并且在顶部被保持在端部4上。用于进行重整工艺的催化剂12被布置在内部重整装置管道11的下端与外部重整装置管道5的下端之间呈杯状的环形空间中。重整装置管道11在内侧上以及在外侧上优选设有肋13，14，所述肋用于在催化剂12与被重整装置管道11所包围的燃烧室15之间进行传热。燃烧器16被配置给燃烧室且被用于加热催化剂12且被设计用以使被引入到燃烧室15中的燃料进行无焰氧化。为此设置大量气体和空气喷嘴17，18，所述喷嘴沿同一方向呈环状对齐进行布置并且形成大容量循。与所述喷嘴环同心地布置的中空的圆柱形引导主体19可有助于进行如图1中的箭头所示的大容量循环。
通过利用废热的预热装置20供给气体喷嘴17以及空气喷嘴18。其部件为管线21，22，所述管线以盘绕的形式传导通过在重整装置管道11上部内形成的排气导管23。按照这种方式，被供应至燃烧室15的燃烧气体以及供给的空气受到预热。从而获得较高的同流换热程度和由此的冷却的排气。优选(1-ΔT2/ΔT1)＞0.8，其中ΔT1是预热装置20的排气导管23的入口与出口之间的排气温差，而ΔT2是在出口处的排气温度与在出口处的新鲜空气温度之间的温差。(1-ΔT2/ΔT1)至少大于0.5。
可以在中心设置用于对燃烧室15进行预热直至开始进行无焰氧化的点火喷嘴Z或电加热装置。
至此所描述的蒸汽重整装置1包括布置在外部同流换热管道5与内部同流换热管道11之间的环形空间10中的蒸汽发生器24并且以热学工艺的方式与所述管道相联接。蒸汽发生器24优选包括盘管，所述盘管被分为多个部段并且相对于预热装置而言同心地进行布置。管道25被布置在中间，其与内部重整装置管道11一起围起另一个环形空间26。在该空间中填充有用于使排气导管23与重整产物导管热绝缘隔开的绝缘材料27，所述重整产物导管在外部重整装置管道5与管道25之间形成穿过所述环形空间10。
蒸汽发生器24具有给水连接装置28，从所述给水连接装置开始，第一盘管部段29引导通过在重整产物出口31处终止的重整产物导管。盘管部段29构成以逆流方式进行工作的水/重整产物逆流散热器。
盘管29通向桥接管道32，所述桥接管道沿轴向引导穿过空间26。随后，引导回到构成重整产物导管的外部环形空间10，并且在那里作为盘管部段33继续延伸。所述盘管构成了水加热器且同时构成了重整产物激冷装置(急冷器，图3和图5中的A段)。可透气的环状绝缘体34被布置在盘管部段33与催化剂12之间，其防止在没有负载时，即在给水流过量为零或接近为零的情况下，蒸汽发生器24产生过热。
另一个盘管部段35紧跟在盘管部段33后面并且包括多条盘管36，38(图3和图5中的B段)。这些盘管36，38已被埋置在催化剂中，所述催化剂填充盘管之间的空间并且构成了后续的反应器。在此，第一盘管36已被埋置在例如CO转化催化剂37中。在本典型实施例中，随后的盘管38(图3和图5中的C段)已被埋置在甲烷生成催化剂39中。催化剂37，39可被附接到适当的催化剂主体上，例如被附接到铁丝网等上，也可作为疏松的大块材料被沉积在盘管36，38之间，或者可作为带有肋的管道被直接成形在蒸发器的肋上。
按照这种方式，蒸发器24被分为A、B、C三段，即用于至少部分地蒸发水和对重整产物进行激冷的盘管部段33，以及由盘管36，38构成的部段，其中在很大程度上完成水的蒸发的另一个部段通过与相应的催化剂37，39进行热交换而设置。催化剂37，39构成了两级后续反应器。
蒸发器的出口通过一条向上的管道41与压力控制阀42相连接，所述压力控制阀保持蒸发器24中的压力恒定，而与从其中通过的流量无关。压力控制阀42排放出的蒸汽被引导至喷射泵44的推进喷嘴连接装置43，其抽吸连接装置45与燃料供应管线相连接。其出口将蒸汽和燃料的混合物供给至供给管线7。
通过给水泵46向给水连接装置28提供给水。控制装置47基于借助温度传感器48检测到的催化剂12的温度对给水泵46进行控制或调节，从而使得催化剂12的温度保持恒定。由于燃烧器和燃料电池对空气的需要量与能量供应PCH4和由此的给水温度成比例，因此鼓风机49的调节比可以简单的方式追踪受控制装置47控制的给水泵46的调节比。
空气和燃烧气体通过管线21，22进行供给。来自燃料电池阳极的残余气体可被用作燃烧气体。
重整产物被传送至燃料电池52的阳极输入端。阳极产生的残余气体经由管线53被传送至预热装置20。鼓风机49将空气传送至燃料电池的阴极和预热装置20。
下面对当前所述的蒸汽重整装置的操作进行描述。
参见图2-4，这里，通过曲线中的分支I，图中示出了经由管线21，22供给的气体的温度，即空气和燃烧气体的温度。曲线中的分支II示出了逆流排出的排气的排气温度。所示出的温度反应出如图4所示的蒸汽重整装置1特别是其同流换热器的温度曲线。图3中曲线的环形分支III表示在进行无焰氧化的过程中燃烧室15内的温度。如图中所示，气体进行多次回转通过燃烧室15。可以注意到，在排气温度为例如150℃时，空气和气体有可能实现预热达到约800℃。
图2中的曲线表示待进行重整和已进行重整的气体的温度曲线。曲线中的分支IV表示对盘管部段29中的给水进行加热的情况，所述盘管部段同时也是给水预热器和水/重整产物逆流式冷却器。现在，处于压力下并且被预热的给水在略高于100℃的温度下被传送至蒸发器24。起初，由曲线中下部水平的分支V表示这一过程。受到预热的给水在点VI处进入蒸发器中。给水在盘管部段33中达到蒸发温度(曲线VIII)，然后给水流过整个蒸发器24，在蒸发器24中给水缓慢地蒸发。在这一过程中，给水保持处于其蒸发温度，例如约200℃，如曲线中的水平分支VIII所示。按照与加热管道相同的方式，管式蒸发器24为后续的反应器设定了均匀的温度。不会超过蒸发温度TS。借助位于压力控制阀42处的蒸发器压力设定蒸发器温度的大小。
即便是在负载发生变化的情况下，特别是在最后阶段中，如图2中所示的温度曲线也保持在较窄的限值范围内。按照这种方式保持后续反应的选择性。在最后的后续反应阶段设定的温度在此仅受到压力控制的影响。
生成的蒸汽从蒸发器24到达喷射泵44。喷射泵44通过推进喷嘴直径与混合喷嘴直径之间的比值固定蒸汽/燃料比。喷射泵44通过其抽吸连接装置45吸出所需量的燃料并将其与蒸汽进行混合。在该过程中，蒸汽温度起初略微降低(图2，曲线中的分支XI)，其中混合燃烧气体的温度突然升高(曲线中的分支X)。然后，该温度缓慢升高直至达到供给连接装置8(曲线中的分支XI)。在催化剂12中，曲线温度根据分支XII继续增高直至已由温度传感器49检测到温度达到TR，并且通过计量给水量而经常进行调节。由催化剂12产生的重整产物使反应器9处于该温度。在遇到蒸发器24(盘管部段33)的第一部段时，重整产物受到激冷(图2，曲线中的分支XIII)，如部段A所示。
此后，冷却的重整产物到达催化剂37和39。在那里，发生后续的CO转化反应。精确的温度控制防止产生太多的甲烷，特别是现有的CO2部分。
当前所述的蒸汽重整装置1本身稳定地工作。电输出Pel的增大的下降幅度恶化了阳极残余气体的卡值。因此，若温度传感器49处的温度下降，那么控制装置就会增强给水传输，且因此增大蒸汽生成量和重整产物生成量。阳极残余气体的增多使得燃烧室15中的燃烧器输出增大。按照这种方式，蒸汽重整装置1自动与负载相匹配。
实际的蒸汽重整装置1已获得以下特征值：
其中V[m3/h]     --标准状态下的容积流量；
Hu[kWh/m3]      --卡值
使用阳极残余气体加热重整装置时生成氢的转化效率为：
×在燃料电池中转化的氢(典型为75％)
新型重整装置的实例：
-外部尺寸：L＝0.6m，D＝0.3m-工艺气体：1m3/h的卡值为10kWh/m3的天然气-水：在15巴下2.5Kg/h(＝3m3/h蒸汽，S/C＝3)-加热气体：0.41m3/h的卡值为10kWh/m3的天然气-重整产物：4m3/h的卡值为3kWh/m3的H2-效率ηR＝85％。
在使用阳极残余气体进行加热时，(25％的H2来自包括在甲烷生成过程中形成的CH4的重整产物)
-可用的氢：2.7m3/h的卡值为3kWh/m3的H2-效率ηR＝81％。
能够受到影响的重整产物的损失是相应成比例的ΔTW(ΔTW为壁部温度与环境温度之间的温差)、ΔT2和ΔTR(参见图2)。这些温度变化值进一步是对于进行无烟重整和转化反应来说必要的重整产物中过量蒸汽的函数。
该新型紧凑型蒸汽重整装置1在一个装置中结合了对天然气或其它燃料进行蒸汽重整，包括对CO进行后续清洗。通过在后续反应器37，39，39a中仔细地进行温度控制而对CO进行受控的催化清洗。借助蒸发器24受到压力控制的工作而有可能实施温度控制。

Claims (19)

1、一种紧凑型蒸汽重整装置(1)，
具有燃烧器(16)，
具有通过燃烧室(15)而被加热且被用于由燃料和H2O蒸汽生成重整产物的反应器(9)，
具有在对排气热量进行回收时对供给空气和/或供给燃料进行预热的预热装置(20)，所述预热装置被连接至燃烧器(16)且其热回收系数(ΔT1/ΔT2)大于0.5，
具有围绕预热装置(20)的环形室(10)，重整产物流过所述环形室并且所述环形室与外部热绝缘，
具有用于在压力下产生H2O蒸汽且被布置在环形室(10)中的管式蒸发器(24)，
具有大量除去生成的重整产物中的一氧化碳部分的后续反应器(37，39，39a)，所述后续反应器同样被布置在环形室中并且与水从其中流过的管式蒸发器(24)形成热连接。
2、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，所述重整产物和水沿相同的流动方向流过后续反应器(37，39，39a)和管式蒸发器(24)。
3、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，水/重整产物逆流式冷却器(29)被连接到管式蒸发器(24)的入口侧和后续反应器(37，39，39a)的出口侧上。
4、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，所述后续反应器(37，39，39a)中含有转化催化剂(37)和/或甲烷生成催化剂(39)和/或后续氧化催化剂(39a)。
5、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，所述管式蒸发器(24)被设计成耐压密封的盘管，所述盘管限定出布置利于进行后续反应的催化剂(37，39，39a)的盘绕空间。
6、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，所述管式蒸发器(24)被实施为耐压密封的带有肋部的管道。
7、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，压力调节装置(42)被连接到管式蒸发器(24)的出口上。
8、根据权利要求7所述的紧凑型蒸汽重整装置，其特征在于，调节压力调节装置(42)达到这样的压力，使得蒸发管道(24)中的水的蒸发温度被设定在130℃与280℃之间。
9、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，在与后续反应器(37，39，39a)形成热连接的区域中，管式蒸发器(24)中的物料流中含有液相。
10、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，喷射泵(44)被连接到管式蒸发器(24)上，所述喷射泵被用于通过抽吸加入燃料并且用于产生供给反应器(9)的H2O蒸汽/燃料混合物。
11、根据权利要求10所述的紧凑型蒸汽重整装置，其特征在于，所述喷射泵(44)是一个未经调节的喷射泵。
12、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，所述反应器(9)与温度传感器(48)相连，所述温度传感器被用于影响管式蒸发器(24)的给水供应量，使得如果温度下降则给水供应量增大，反之亦然。
13、根据权利要求12所述的紧凑型蒸汽重整装置，其特征在于，所述温度传感器(48)控制用于向燃烧器(16)供给燃烧空气的鼓风机(49)。
14、根据权利要求1所述的紧凑型蒸汽重整装置，其特征在于，所述燃烧器(16)被至少部分地供给来自连接好的燃料电池(52)的阳极的残余气体。
15、一种用于通过蒸汽重整装置对燃料进行蒸汽重整的方法，所述蒸汽重整装置具有用于在压力下产生H2O蒸汽的蒸发器(24)和连接到蒸发器(24)上的喷射泵(44)，其中在蒸发器(24)中产生的蒸汽作为推进剂被供应至喷射泵(44)，其中借助通过抽吸而加入燃料，H2O蒸汽/燃料混合物被生成用于供给反应器(9)。
16、根据权利要求15所述的方法，其特征在于，通过与后续反应器(37，39，39a)形成热接触而加热蒸发器(24)，所述后续反应器被用于大量除去生成的重整产物中的一氧化碳部分。
17、根据权利要求15所述的方法，其特征在于，所述蒸发器(24)的工作是通过对其压力进行调节而进行的。
18、根据权利要求17所述的方法，其特征在于，在所述蒸发器(24)的工作过程中，所述蒸发器的压力保持恒定。
19、根据权利要求15所述的方法，其特征在于，通过对被供应至蒸发器(24)的给水量进行调节而对蒸发器(24)的输出进行调节。
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