CN1481268A - 改进的氢和二氧化碳联产品 - Google Patents

改进的氢和二氧化碳联产品 Download PDF

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CN1481268A
CN1481268A CNA018209157A CN01820915A CN1481268A CN 1481268 A CN1481268 A CN 1481268A CN A018209157 A CNA018209157 A CN A018209157A CN 01820915 A CN01820915 A CN 01820915A CN 1481268 A CN1481268 A CN 1481268A
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gas
tail gas
stream
unit
preparation facilities
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CN1240459C (zh
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S·雷迪
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Fluor Corp
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  • Separation Of Gases By Adsorption (AREA)
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  • Vaporization, Distillation, Condensation, Sublimation, And Cold Traps (AREA)
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Abstract

气体制备装置(100)具有接收原料气(120)并制备第一尾气流(132)和第一产物流(134)的第一分离器(130)，和接收第一尾气流(132)并制备第二产物流(142)和第二尾气流(144)的第二分离器(140)。液化单元(150)接收至少部分第一产物流(134)和至少部分第二尾气流(144)，并制备第三产物流(154)和第三尾气流。第三尾气流的第一部分(152A)与第一尾气流(132)结合，而第三尾气流的第二部分(152B)用作非尾气。在运行气体制备装置(100)的方法中，PSA单元用作第二分离器(140)，氢作为第二产物流(142)收集，而解吸的气体作为第二尾气流(144)排放。

Description

改进的氢和二氧化碳联产品
发明领域
本发明的领域是同时制备氢和二氧化碳。
发明背景
诸如炼油厂气或燃烧过程的尾气的气体的复杂混合物常常在净化气的制备中用作原材料，而且开发了各种系统，以较高纯度(即大于90％(v/v))从单一气体混合物中同时分离出至少两种或多种气体。
某些系统采用PSA单元的串联结构，其中第一PSA单元与第二PSA单元具有不同的选择性，且第一单元排出的尾气直接导向第二PSA单元的进料端。这种结构的实例描述在R.Kumar的US 4913709中。在一次要净化较大体积尾气的情况下，Kumar的带有不等吸附特性的吸附床的PSA单元的串联结构是有利的。然而，由于吸附剂床的不同物理-化学性能，往往增加了交叉循环步骤的复杂程度和数量，从而不利地增加了造价和维护要求。
其他系统利用具有PSA单元和非PSA单元的结构，如Fuderer的US 4553981中描述的。在Fuderer的系统中，二氧化碳作为尾气通过CO2洗涤器从原料气流中除去，随后将除去CO2的气流送入H2-PSA单元中。然后将H2-PSA尾气通过尾气管排到大气中，或回收到转化炉或变换(Shift)单元中。当从进料气体中同时分离H2和CO2时，可有益地采用Fuderer的结构，从而通过将尾气回收到变换炉的重整装置中，减少来自洗涤器和H2-PSA单元的尾气中的氮和/或氩的不想要的聚积。然而，在回收回路中仍存在相当数量的二氧化碳和氢，一般都被排出或燃烧掉，使它们不再适于回收。
其它系统采用选择性膜，以从PSA单元的尾气中分离出所想要的气体组分。例如G.Intille在US4229188中描述了用氢可透过性膜从PSA单元的尾气中回收H2。Instille的膜以高选择性在单一处理步骤中除去H2，然而应用这种膜通常要求较高的压力，从而增加了总体能量要求。为了避免与氢可透过膜相关的至少某些问题，Anand等在US5435836中提出使用吸附剂膜。吸附剂膜一般能以较高的专一性在相对低的压力下回收氢。然而较低压力的优点会被膜交换的需要所抵消，从而增加氢装置的复杂性，或需要不连续的操作。
这样，尽管本领域已知从气体混合物中同时制备所想要的气体的各种系统，但是所有或几乎所有系统都存在一个或多个缺点。因此，需要提供改进的用于从气体混合物中同时制备所想要气体的方法和装置。
发明概述
本发明涉及包含气体源、第一和第二分离器，以及液化单元的气体制备装置。第一分离器接收来自气体源的原料气，并产生第一尾气流和第一产物流，而第二分离器接收第一尾气流，以产生第二尾气流和第二产物流。液化单元接收第一产物流和第二尾气流，从而产生液化的第三产物流和第三尾气流，而且至少部分第三尾气流与第一尾气流混和。
在本发明主题的一个方面，气体源提供主要含有氢和二氧化碳的原料气，它通过蒸汽重整过程由天然气制备。而第一分离器优选包括CO2洗涤器，第二分离器包括氢变压吸附(PSA)单元，而液化单元在其尤其优选的方面包括自冷单元。
在本发明主题的另一个方面，从原料气中除去第一气体组分和第二气体组分的方法采用PSA单元，其产生主要含有第二气体组分的第一产物流，和主要含有第一气体组分和第二气体组分的第一尾气流。将至少部分尾气流送入液化单元中，以产生第二产物流和第二尾气流，且至少部分第二尾气流返回PSA单元。
本发明的各种目的、特征、方面和优点将从本发明的以下优选实施方式的详细描述，以及附图中变得更明显。
附图简述
图1是根据本发明的主题的气体制备装置的示意图。
图2是描述根据本发明主题改善从原料气中回收气体组分的方法的流程图。
发明详述
本文所用术语“非尾气”指用在除排放到大气中以外的方法中的气体，优选的方法是包括在蒸汽重整炉或燃气轮机中燃烧、膨胀或压缩，以及在热交换装置中加热/冷却。
同样用于本文的术语“自冷系统”指用CO2作为制冷剂制备高纯度液态CO2的装置。尤其可作考虑的自冷系统描述在S.Reddy的PCT申请PCT/US99/00087中，本文参考引用该文献。
本文另外使用的术语“H2-PSA单元”和“氢PSA单元”均指设置为制备主要含有氢的产物气流的PSA单元。同样，“CO2-PSA单元”和“二氧化碳PSA单元”指设置为制备主要含有二氧化碳的产物气流的PSA单元，其中术语“主要含有”指该产物气流含有至少50％二氧化碳、氢或主要存在于一种产物中的其他化合物。
在图1中，装置100通常带有气体源110，其中原料气流112在重整炉114中重整，并通过输送管116输送到转化炉118中，经重整的原料气在其中转化成原料气流120。第一分离器130从原料气除去第一气体组分，产生第一产物流134和第一尾气流132。将第一尾气流132送入第二分离器140中，产生第二产物流142和第二尾气流144。将第二尾气流144和第一产物流134都送入液化单元150中，第三产物流154从液化单元中除去已液化的产物。离开液化单元的第三尾气流的第一部分152A与第一尾气流132混和，而第三尾气流的第二部分152B在重整燃烧炉中燃烧。
在本发明主题的优选方面中，生产装置是用于氢和二氧化碳联产的装置，其中第一气体组分为二氧化碳，而第二气体组分为氢。该气体源包括蒸汽重整炉和变换炉，以将主要含有CH4的天然气流转化成主要含有CO2和H2的原料气流。第一分离器是与闪蒸单元和从原料气中除去第一部分CO2的分离罐联用的CO2洗涤器，从而制备CO2浓度大于80mol％的第一产物流，和送入氢PSA单元的第一尾气流。第二分离器是制备含有纯度大于99mol％的H2的第二产物流，以及含有约20mol％H2和大于70mol％的CO2的第二尾气流的氢PSA的单元。第一产物流134和第二尾气流144均送入自冷单元150中，以产生含有纯度大于98mol％的CO2的第三产物流154。约70％(体积)的第三尾气流(即第三尾气流的第一部分)与第一尾气流混和，而约30％(体积)送入蒸汽重整燃烧炉中(即第三尾气流的第二部分)。
对于液化单元的结构，应特别注意的是，通过(a)将H2-PSA尾气送入自冷单元和(b)同时将自冷单元尾气回收到H2-PSA中，可提高CO2和H2的回收速度。例如，在第一分离器中未从原料气流除去的CO2将与H2一起，通过来自H2-PSA单元的第二尾气流送入自冷单元中。第二尾气流中的CO2在自冷单元中从第二尾气流中深冷回收，使自冷单元成为第二分离器。第二尾气流中的H2流经自冷单元，并将至少部分第三尾气流再次送入H2-PSA中，来自第二尾气流的H2循环至H2-PSA单元并随后回收。
还应注意到，在本发明主题的可选择的方面中，尽管气体源不必限于含有蒸汽重整器和变换炉的气体源，但还可包括各种其他组分，这种选择主要在于所想要的气体。例如，在特别需要氢产物的场合，合适的气体源可采用用于各种烃的部分氧化或煤的气化的组分。另一方面，气体源不必局限于主要制备氢的气体源，还可包括制备N2、CO2、CO、He、Ar等的气体源。在较纯的气体为工业过程的副产品的情况下，还可进一步考虑的是，合适的气体源还可含有在除产物外的气体净化，如PSA单元、吸收剂单元、蒸馏塔、酸性气体去除单元等中应用的元素。
因此，原料气体流不必限于主要含有H2和CO2的气体混合物。或者，原料气流可尝试包括含有C2-C6烃和更高级的烃(它们可以是或不是脂族的)，诸如N2、He、Ar的惰性气体的气体混合物，或已富化或贫化了一种或多种化合物的预处理的气体混合物。例如，可考虑的原料气流可包含来自蒸汽重整过程、部分氧化法、汽提过程、燃烧或煤气化过程的尾气。
对于第一分离器，优选的合适的第一分离器包括酸性气体去除单元，尤其可考虑的酸性气体去除单元采用除去至少部分第一气体组分的溶剂。取决于特定的气体组分和分离器结构，溶剂可包括物理和化学溶剂，优选的溶剂是一乙醇胺、活化的甲基-二乙醇胺、丙二醇和乙二醇二甲醚。尽管优选的第一分离器包括与闪蒸单元和分离罐联用的CO2洗涤器，但也可考虑各种作为选择的分离器。例如，在处理较少体积的原料气体时，作为选择的第一分离器可包括选择性膜。在由深冷过程产生原料气体的其他情况下，可利用蒸馏装置作为第一分离器，而在要求以高纯度(如大于99％(v/v))回收气体组分的过程中，可用变压吸附单元作为第一分离器。同样，第二分离器不必限于氢PSA单元，作为选择，第二分离器可包括CO2-PSA单元、选择性膜、蒸馏装置等，只要可选择的第二分离器与第一分离器在流动上联结，并接收至少部分第一尾气流即可。
尽管优选的液化单元是二氧化碳自冷单元，但作为选择的可考虑的液化单元也可包括带有要求诸如氨、氟代烃或氟氯烃的外部制冷剂的过程的液化单元。由自冷单元获得的液化CO2优选具有大于98％(v/v)，更优选的大于99％(v/v)，最优选的大于99.9％(v/v)的纯度。对于与第一尾气流混和的第三尾气流的量/份额，可以考虑的是，尽管约70％(v/v)是优选的，但许多其他量/份额也是合适的，只要至少部分第三尾气流回到第二分离器中即可。通常考虑的量/份额范围为0.1％-100％，更优选的量/份额为40-80％。例如，在第三尾气流仅含有少量氢，且第二分离器为H2-PSA单元的情况下，约5-25％的量可回到第一尾气流中。另一方面，在许多H2-PSA单元的常规操作期间，第二尾气流将含有约20％(v/v)的氢，其通过将70-90％(v/v)或更多的第三尾气流返回到第一尾气流，可将这些氢几乎完全回收。此外，应该注意的是，第三尾气流的第一部分与第一尾气流的混和可以是连续的或不连续的过程。例如，在某些情况下，80％的第三尾气流可连续地混和到第一尾气流中，而在其他情况下，100％的第三尾气流可以在60秒的间隔中用50秒与第一尾气流混和。
同样，第二部分的第三尾气流的量/份额可与优选的量/份额不同，一般取决于第一部分的第三尾气流的量/份额。对于第二部分的第三尾气流的用法，只要将第二部分第三尾气流作为非尾气利用，除在蒸汽重整炉中燃烧外的各种用途也是合适的。例如，在第二部分第三尾气流具有较低温度的情况下，第二部分可作为冷却剂使用，或在可燃烧组分(如甲烷)的量较高的情况下，第二部分可在燃气轮机中燃烧。应该注意的是，由于第一和第二分离器与液化单元协同操作的结构，第一和第二气体组分的浓度优选低于10％(v/v)，更优选低于1％(v/v)，最优选低于0.1％(v/v)。
在图2中，从原料气中去除第一和第二气体组分的常用方法200具有步骤210，其中提供了从原料气中去除至少一部分第二气体组分，从而产生主要含有第二气体组分的第一产物流，和主要含有第一气体组分和第二气体组分的第一尾气流的PSA单元。在另外的步骤220中，将至少部分第一尾气流送入液化单元中，以除去至少一部分第一气体组分，从而制备第二产物流和第二尾气流，而在更进一步的步骤230中，至少部分第二尾气流返回到PSA单元中。
在本发明主题的优选方面，第一和第二气体组分分别为二氧化碳和氢，并通过变换炉中的蒸汽重整和处理而由天然气获得原料气(主要含有H2和CO2)。该PSA单元是制备主要含有H2的第一产物流，以及主要含有H2和CO2的尾气流的H2-PSA。将PSA尾气送入二氧化碳自冷单元中，通过液化从该尾气中除去CO2，从而制备液化的二氧化碳产物流。将来自自冷单元的约70％(v/v)已除去CO2的尾气返回到PSA单元的进料端。
特别应该注意的是，根据本发明内容的方法对从原料气中除去第一和第二气体组分的方法给予了多方面的优点。例如，通过将来自H2-PSA单元的尾气送入二氧化碳自冷单元中，来自原料气的剩余二氧化碳得到有效回收。此外，来自自冷单元的至少一部分尾气中途返回到H2-PSA单元中，显著减少了作为尾气的氢的损失。这样，尝试的方法有效地提高了对来自原料气的第一和第二气体组分的回收。
对于方法200与气体制备装置100间的相应部件，相同的考虑应用于装置100中讨论的方法200中的部件(参见上文)。
这样，本文公开了用于改善的共同制备氢和二氧化碳的方法和装置的具体实施方式和应用。然而对于本领域普通技术人员很明显的是，除本文已描述的以外的更多修正也是可能的，而不会脱离本发明的概念。因此本发明的内容并不受限制，只要在附属权利要求的精神内。而且，在说明书和权利要求的解释中，所有术语应以与内容一致的尽可能宽的方式解释。具体说，术语“包含”和“包括”应以非排他性方式解释为指部件、组分或步骤，即指参考的部件、组分或步骤可以存在或利用，或与未参考表述的其他部件、组分或步骤结合。

Claims (18)

1.气体制备装置，包含：
提供含有第一气体组分和第二气体组分的原料气流的气体源；
与气体源流动联结的第一分离器，其中第一分离器除去原料气流中的至少部分第一气体组分，从而产生第一尾气流和主要含有第一气体组分的第一产物流；
与第一分离器流动联结的第二分离器，其中第二分离器除去第一尾气流的至少一部分第二气体组分，从而产生第二尾气流和主要含有第二气体组分的第二产物流；
与第一和第二分离器流动联结的液化单元，其中液化单元接收至少部分第一产物流和至少部分第二尾气流，从而产生主要含有液化的第一气体组分的第三产物流；和
其中液化单元产生第三尾气流，第三尾气流的第一部分与第一尾气流结合，而另一部分用作非尾气。
2.权利要求1的制备装置，其中原料气流包含来自蒸汽重整过程的尾气。
3.权利要求1的制备装置，其中原料气流包含来自部分氧化过程和煤气化过程之一的尾气。
4.权利要求1的制备装置，其中第一气体组分为二氧化碳。
5.权利要求1的制备装置，其中第二气体组分为氢。
6.权利要求1的制备装置，其中第一分离器包含酸性气体去除单元。
7.权利要求6的制备装置，其中酸性气体去除单元应用除去至少部分第一气体组分的溶剂。
8.权利要求7的制备装置，其中溶剂选自单乙醇胺、活化的甲基-二乙醇胺、丙二醇和乙二醇二甲醚。
9.权利要求1的制备装置，其中第二分离器包含变压吸附单元。
10.权利要求9的制备装置，其中变压吸附单元为氢变压吸附单元。
11.权利要求1的制备装置，其中液化单元包含二氧化碳自冷单元。
12.权利要求1的制备装置，其中第三尾气流的第二部分作为非尾气的应用包括在重整炉中燃烧。
13.权利要求1的制备装置，其中第三尾气流的第二部分作为非尾气的应用包括在燃气轮机中燃烧。
14.从原料气中除去第一气体组分和第二气体组分的方法，包括：
提供PSA单元，其从原料气中去除至少部分第二气体组分，从而产生主要含有第二气体组分的第一产物流，和主要含有第一气体组分和第二气体组分的第一尾气流；
将至少部分第一尾气流送入液化单元中，以除去至少部分第一气体组分，从而产生第二产物流和第二尾气流；和
将至少部分第二尾气流循环回PSA单元中。
15.权利要求14的方法，其中第一气体组分为二氧化碳。
16.权利要求14的方法，其中第二气体组分为氢。
17.权利要求14的方法，其中PSA单元包含氢-PSA单元。
18.权利要求14的方法，其中液化单元包含自冷单元。
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