CN100347077C - 从含甲烷的气体特别是天然气中获得氢的方法,和实施该方法的装置 - Google Patents

从含甲烷的气体特别是天然气中获得氢的方法,和实施该方法的装置 Download PDF

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CN100347077C
CN100347077C CNB2004800216034A CN200480021603A CN100347077C CN 100347077 C CN100347077 C CN 100347077C CN B2004800216034 A CNB2004800216034 A CN B2004800216034A CN 200480021603 A CN200480021603 A CN 200480021603A CN 100347077 C CN100347077 C CN 100347077C
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M·布鲁曼菲尔德
V·刘
B·米尔克
M·米歇尔
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Abstract

本发明涉及从含甲烷的气体，特别是天然气中获得氢的方法。在重整装置(4)中，借助于水蒸气将在所述气体中所含有的烃催化裂解成氢、一氧化碳和二氧化碳。在随后串联的转化阶段中，使用水蒸气将所产生的一氧化碳催化转化成二氧化碳和水。通过气体洗涤步骤(7)将二氧化碳从转化的气体流(8)中去除，随后将经洗涤的富含氢的气体流(10)在压力变化吸附装置(11)中分离成由氢组成的产物气流(12)和废气流(13)。将废气流(13)与在气体洗涤步骤之后从气体流(10)中分出的氢(14)一起作为几乎不含碳的燃气引入重整装置(4)中，并在那里燃烧。本申请的目标还涉及用于实施该方法的装置。

Description

从含甲烷的气体特别是天然气中获得氢的方法，和实施该方法的装置
本发明涉及从含甲烷的气体，特别是天然气中获得氢的方法。
从US 5 131 930中可知一种常规的制氢装置，其用天然气作为使用材料进行运作。在该装置中，首先在一个加热的重整装置中，进行通常用水蒸气推动的天然气中含有的烃的催化裂解，以生成一氧化碳和含氢的合成气。然后，将一氧化碳催化转化成氢，并随后借助于一个压力变化吸附装置进行氢的提纯。将吸附装置的废气输回重整装置的燃烧室中，并在那里与另外引入的天然气一起进行燃烧。还已知，使用炼厂气或其他燃气作为另外的燃料。通过甲烷的蒸汽裂解，根据水煤气平衡
CO+H2O＝>H2+CO2
可产生显著数量的二氧化碳，二氧化碳的数量在转化阶段中通过一氧化碳转化而进一步提高至通常大约16体积％(干燥的)的浓度。这一数量的二氧化碳通过燃烧室的烟囱与经燃烧另外的含碳燃料而产生的二氧化碳一起释放到大气中。烟气中的CO2含量通常超过20体积％(干燥的)。因此，在精炼厂中，一个如此设计的制氢装置是最大的二氧化碳释放者之一。
从US 4 553 981中可知一种获得氢的方法，在该方法中将含烃的气体用蒸汽进行重整和转化。然后，在洗涤步骤中，从转化的气体流中分离出CO2废气流。随后，借助于压力变化吸附装置进行氢的分离。压缩吸附装置的废气流，并输回重整或转化过程中。由此产生大的循环流。为了避免惰性气体如氮气的聚集，必须从压力变化吸附装置的废气流中获取清洗气流。以常规方式点燃重整装置。此外，该方法是费力和昂贵的。
本发明的任务在于，给出一种简单而且成本低的用于从含甲烷的气体特别是天然气中获得氢的方法，在该方法中只有少量的二氧化碳释放到环境中。
本发明的方法和这一任务的解决方案是从含甲烷的气体特别是天然气中获得氢的方法。在重整装置中，借助于水蒸气将在所述气体中含有的烃催化裂解成氢、一氧化碳和二氧化碳，并在随后串联的转化阶段中，使用水蒸气将所产生的一氧化碳催化转化成二氧化碳和氢。通过气体洗涤步骤将二氧化碳从转化的气体流中去除，随后将经洗涤的富含氢的气体流在压力变化吸附装置中分离成由氢组成的产物气流和废气流。将废气流与在气体洗涤之后从气体流中分出的氢一起作为几乎不含碳的燃气引入重整装置中，并在那里燃烧。
于在重整装置中将烃几乎完全裂解成氢、一氧化碳和二氧化碳的同时，随后在转化阶段中将产生的一氧化碳转变成二氧化碳，并在随后的气体洗涤步骤中将这些二氧化碳去除。因此，压力变化吸附装置的废气主要含有氢气和只有很少量的碳。在气体洗涤之后从气体流中分出的氢也是这样的情况。因此，在这两个气体流于重整装置中同时燃烧的过程中，产生主要由氮气和水组成的废气，而二氧化碳的含量是低的。通过这种气体回流而取消了使用含碳的燃料所进行的重整装置的辅助燃烧，从而明显减少了二氧化碳的释放。与常规的方法相比，二氧化碳的排放减少大约75％。在本发明的教导的范围内所使用的方法技术步骤无例外地都是成熟的技术，这些技术已经在氢气制备中卓有成效地使用了较长时间。对于达到所述二氧化碳减少所需的花费是比较低的。因此，还存在这样的可能性，即改装现有的常规制氢装置，以便用其运行本发明的方法。
优选地，对于转化阶段使用在中等温度下运行的转化反应器，或者使用其后串联有低温转化反应器的高温转化反应器。由此，保证了将产生的一氧化碳几乎完全转化成二氧化碳，这些二氧化碳可以随后通过气体洗涤而从气体流中去除。使用随后串联的低温转化反应器具有这样的优点，即能够继续利用现有制氢装置的高温转化反应器，由此明显降低了现有装置的改装成本。
优选地，在气体洗涤步骤中分离出工业纯的二氧化碳，其用于工业用途，或者进一步加工成具有食品工业中可用的质量的产物。除了作为食品工业的使用材料进行使用之外，例如还可以考虑作为有效开采石油的措施将工业纯的二氧化碳用于填充石油钻井。作为另一种选择，还可以将二氧化碳用作甲醇合成的原料。在此，二氧化碳的洗涤可以用已知的物理方法来进行，例如甲醇吸收法(Rectisol)、聚乙二醇二甲醚吸收法(Selexol)或Genosorb，或者用化学或物理/化学方法来进行，例如aMDEA(N-甲基二乙醇胺的水溶液)或环丁砜法(Sulfinol)。
如果要将现有的制氢装置改装成符合最小化CO2的目的，那么合适的是将转化的气体流在进入待重新构建的CO2洗涤步骤中之前进行压缩，以便平衡经洗涤产生的压力损失。由此，提高CO2洗涤步骤的效果。
本发明的目标还涉及用于实施本方法的装置，其具有至少一个配备有燃烧室的重整装置，以用于将气态的烃用水蒸气催化裂解；使用至少一个转化反应器的转化阶段，以用于将一氧化碳用水蒸气催化转化成二氧化碳和氢；用于从离开转化阶段的气体流中分离出二氧化碳的气体洗涤步骤；和随后串联的用于分离氢的压力变化吸附装置，在其上连接着返回燃烧室的气体管道，以便用从吸附装置中出来的气体流点燃重整装置；其中，设定一个附加的装置，以用于将离开气体洗涤步骤的富含氢的气体流的一部分输回重整装置的燃烧室中。该装置的优选实施方案包括转化阶段包含在中等温度下运行的转化反应器，或者其后串联有低温转化反应器的高温转化反应器；以及在气体洗涤步骤的二氧化碳出口之后连接有用于提浓分离出的二氧化碳的纯化阶段。
在下文中，将依据仅仅描述了一个实施例的附图来详细地解释本发明。附图示意性地表示：
图1本发明方法的线路框图，
图2在改装常规制氢装置之后的本发明方法的线路框图。
图1显示了用于从含甲烷的天然气中获得氢的本发明方法。向天然气流1中混入水蒸气流2。在一个配备有燃烧室3的重整装置4中，借助于所混入的水蒸气流2将在天然气中含有的烃特别是甲烷催化裂解成氢、一氧化碳和二氧化碳。该重整过程进行得几乎完全，从而在重整装置4的出口处实际上不再存在含烃的气体。在随后串联的、于中等温度下运行的转化反应器5中，借助于水蒸气将所产生的一氧化碳催化转化成二氧化碳和氢。这一反应也进行得几乎完全，以致于从转化反应器5中出来的气体流8的一氧化碳含量小于1体积％(干燥的)。随后，通过气体洗涤步骤7，将所产生的二氧化碳几乎完全从气体流8中去除。在该实施例中，洗涤步骤7是用N-甲基二乙醇胺的水溶液(aMDEA)作为洗涤液来进行的。但是，在本发明的范围内，还包括使用其他已知的洗涤方法，例如甲醇吸收法、聚乙二醇二甲醚吸收法、Genosorb或环丁砜法。在进一步的纯化阶段9中，将在洗涤步骤7中所获得的二氧化碳18进一步提浓至食品工业中可用的纯度。经洗涤的气体流10只含有非常少量的碳，并随后在压力变化吸附装置11中将其分离成由氢组成的产物气流12和废气流13。产物气流12具有大于99体积％的氢含量。废气流13同样也主要含有氢，和只是微小数量的不反应或只部分反应的烃。与在洗涤步骤7之后经过装置19分出的、同样也主要由氢组成的部分流14一起，将废气流13通过管道17引入重整装置4的燃烧室3中，并在那里燃烧。在此，如此调节部分流14的量，即在与废气流13共同燃烧时能满足重整装置4的能量需求。因为不仅废气流13而且部分流14均主要由氢组成并只含有少量的碳，燃烧室4的废气15具有高的水蒸气含量和只有低的二氧化碳含量。在常规的获得氢的方法中，燃烧室需要用含碳的燃料，例如天然气和含烃的废气点燃，因此，与之不同，本发明方法的特征在于低的二氧化碳释放。
所述的在本发明的教导的范围内所使用的方法步骤全部都是在技术上成熟的技术，这些技术不仅在制备氢中而且在生产氨中都证明是行之有效的。只是，重整装置4必须具有足够大的尺寸，以便在CO2洗涤之后保证包括燃气供应在内的H2生产。转化反应器5在中等温度下运行，以便确保将所产生的一氧化碳几乎完全地转化成二氧化碳。在该实施例中经纯化阶段9所获得的二氧化碳21可以在食品工业中进行进一步加工。但是，作为另一种选择，对此还存在一种可能性，即将在洗涤步骤7中所获得的工业纯的二氧化碳18直接用于工业用途。在此，例如可以考虑作为有效开采石油的措施填充石油钻井，或者用作甲醇合成的原料。
对于实施所述方法的花费是比较低的。特别地，存在这样的可能性，即改装现有的常规制氢装置，从而可以用其运行本发明的方法。图2显示了根据本发明改装的常规制氢装置。已经存在的装置组件用实线标示，而在改装的范畴内添加的部件用虚线描绘。常规的制氢装置具有一个配备有燃烧室3′的重整装置4′，以用于将气态的烃用水蒸气催化裂解。在这之后，布置有一个高温转化反应器5′，以用于将一氧化碳用水蒸气催化转化成二氧化碳和氢。随后是用于从转化的气体流8′中分离出氢12′的压力变化吸附装置11′，在其上连接着导向燃烧室3′的气体管道17′，以便为了用从吸附装置11′中出来的废气流13′点燃重整装置4′。在改装的范畴内，重整步骤的容量通过一个在重整装置4′之前串联的前重整装置4″以及一个在重整装置4′之后串联的后重整装置4”’而提高了大约20％。但是，可选地，只设定使用这两个重整装置4″、4”’中的一个也是足够的。对于通常在360-500℃的温度下工作的高温转化反应器5′补充一个随后串联的、在大约210-270℃的温度下工作的低温转化反应器5″，以便将一氧化碳尽可能完全地转化成二氧化碳。作为另一种选择，对此还可以用在中等温度下工作的转化反应器来代替存在的高温转化反应器5′。在转化阶段和压力变化吸附装置11′之间，设定一个用于压缩气体流6′的气体压缩机16′以及一个用于分离所产生的二氧化碳18′的气体洗涤步骤7′，其中，在该实施例中将在气体洗涤步骤7′中所获得的二氧化碳18′直接导向工业应用。在气体洗涤步骤7′和压力变化吸附装置11′之间，设定一个附加的装置19′以用于将离开气体洗涤器的富含氢的气体流10′的一部分14′输回重整装置4′、4″、4”’的燃烧室3′、3″、3”’中。最后，使现有的重整装置4′适应现在富含氢的燃料的燃烧以及废热利用。不再使用用于将含烃的燃气引入重整装置4′的燃烧室3′中的现有的气体管道20。图2中的图显示了，用相对较少的花费可将常规的制氢装置如此进行改装，从而可以用其来运行本发明的方法。由此，进一步提高了本发明方法的吸引力。

Claims (7)

1.从含甲烷的气体中获得氢的方法，
其中，在重整装置(4)中，借助于水蒸气将在所述气体中所含有的烃催化裂解成氢、一氧化碳和二氧化碳，并在随后串联的转化阶段中，使用水蒸气将所产生的一氧化碳催化转化成二氧化碳和氢，
其中，通过气体洗涤步骤(7)将二氧化碳从转化的气体流(8)中去除，随后将经洗涤的富含氢的气体流(10)在压力变化吸附装置(11)中分离成由氢组成的产物气流(12)和废气流(13)，和
其中，将废气流(13)与在气体洗涤步骤(7)之后从气体流(10)中分出的氢(14)一起作为几乎不含碳的燃气引入重整装置(4)中，并在那里燃烧。
2.根据权利要求1所述的方法，其特征在于，对于转化阶段使用在中等温度下运行的转化反应器(5)，或者使用其后串联有低温转化反应器(5″)的高温转化反应器(5′)。
3.根据权利要求1或2所述的方法，其特征在于，在气体洗涤步骤(7)中分离出工业纯的二氧化碳(18)，其用于工业用途，或者进一步加工成具有食品工业中可用的质量的产物(21)。
4.根据权利要求1所述的方法，其特征在于，所述含甲烷的气体是天然气。
5.用于实施根据权利要求1-4中任一项所述的方法的装置，其具有
-至少一个配备有燃烧室(3)的重整装置(4)，以用于将气态的烃用水蒸气催化裂解，
-使用至少一个转化反应器(5)的转化阶段，以用于将一氧化碳用水蒸气催化转化成二氧化碳和氢，
-用于从离开转化阶段的气体流(8)中分离出二氧化碳的气体洗涤步骤(7)，和
-随后串联的用于分离氢(12)的压力变化吸附装置(11)，在其上连接着返回燃烧室(3)的气体管道(17)，以便用从吸附装置中出来的气体流点燃重整装置，
其中，设定一个附加的装置(19)，以用于将离开气体洗涤步骤(7)的富含氢的气体流(10)的一部分(14)输回重整装置(4)的燃烧室(3)中。
6.根据权利要求5所述的装置，其特征在于，转化阶段包含在中等温度下运行的转化反应器(5)，或者其后串联有低温转化反应器(5″)的高温转化反应器(5′)。
7.根据权利要求5或6所述的装置，其特征在于，在气体洗涤步骤(7)的二氧化碳出口之后连接有用于提浓分离出的二氧化碳(18)的纯化阶段(9)。
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