CN105723172B - 用于生产co和co2的方法和设备 - Google Patents

用于生产co和co2的方法和设备 Download PDF

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CN105723172B
CN105723172B CN201480062938.4A CN201480062938A CN105723172B CN 105723172 B CN105723172 B CN 105723172B CN 201480062938 A CN201480062938 A CN 201480062938A CN 105723172 B CN105723172 B CN 105723172B
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carbon dioxide
stream
unit
hydrogen
carbon monoxide
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CN105723172A (zh
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A·赫尔南德斯
P·泰里安
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LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude
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LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude
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Abstract

本发明提供一种从含有二氧化碳、氢气和一氧化碳的进料气体生产至少二氧化碳和一氧化碳的方法，此方法包括：通过部分冷凝和/或蒸馏从已压缩的进料气体分离出至少一部分二氧化碳，得到二氧化碳产物和贫二氧化碳料流(7)；贫二氧化碳料流在处理单元(S)中进行处理，得到含有一氧化碳和氢气的进料流(15)，此进料流含有与贫二氧化碳料流相比更少的二氧化碳；和将至少一部分的含有一氧化碳和氢气的进料流加入在深冷温度下操作的分离单元(HYCO)，从而得到一氧化碳产物。

Description

用于生产CO和CO2的方法和设备
本发明涉及用于生产CO和CO2的方法和设备。
“生产CO”应当理解为表示生产含有至少40摩尔％或至少60摩尔％或至少90摩尔％一氧化碳的液态或气态料流。此料流可以含有至多60摩尔％的氢气或至少50摩尔％的氢气。
“生产CO2”应当理解为表示生产含有至少60摩尔％二氧化碳的液态或气态料流。
水蒸气甲烷重整装置能生产纯氢气、以及CO或它们的组合物或混合物。出于环境原因或其它经济原因，越来越重要的是在新项目中包括能捕获的计划和包括捕获CO2的操作。对于氢气生产设备例如SMR设备的情况，也是如此。
本发明涉及简化和优化的方法，其能从来源例如氢气生产装置或其它合适来源例如高炉来生产CO和CO2。
US-A-2012/0121497A描述了一种能有效地从SMR设备捕获CO2的方案：
·使用高温变换、然后进行低温变换，
·通过变压吸附(PSA)分离经变换的合成气，
·压缩PSA尾气，
·通过低于环境温度的提纯单元(CPU)分离CO2，
·使用两组膜以将部分氢气循环到PSA和将部分CO2循环到深冷提纯单元。
EP-A-1869385描述了在PSA中分离以除去氢气，然后进行压缩和低于环境温度的分离。
通常，当在项目中要求共同生产CO时，CO是在高温变换之前从合成气制得的，如US-A-4861351所述。在生产CO和捕获CO2的情况下，明显的解决方式将是使得一部分合成气在变换之前用CO冷箱处理，并将另一部分合成气通过两组变换进行处理(HT变换(Shift)，然后LT变换)，并且CPU位于PSA尾气的路径上。
建议改变在基本包括CO2捕获操作的体系中生产CO的位置，其中从CPU的贫CO2气体制备CO，或可以从用于分离CPU的贫CO2气体的膜的残余物制备CO。根据本发明的方法的一个例子将包括：
·压缩含有氢气、二氧化碳和一氧化碳的进料气体，其是PSA尾气，
·通过深冷提纯单元(CPU)分离CO2，
·处理CPU的贫CO2气体以得到进料气体，其含有一氧化碳和氢气和可能的甲烷作为主要组分，
·使得进料气体进行深冷分离以得到一氧化碳。
处理贫CO2气体的一种方式是：
·使用两组膜，从而将一部分氢气循环到PSA和将一部分CO2循环到深冷提纯单元，
·处理第二个膜的残余物以得到用于深冷分离的进料气体(通常是胺吸收体系以除去CO2，随后可以是吸附体系，用于吸附任何残余CO2)。
进料气体可以如下生产：采用高温(HT)变换，然后通过变压吸附(PSA)分离已变换的合成气，从而形成作为PSA尾气的进料气体，和富氢产物。
在这种情况下，HT变换的入口温度可以基本上调节以保持在CO冷箱中生产CO的实际量。
此方法提供了生产CO和生产CO2的优化整合。尤其是，此方法显著降低了CO深冷分离设备的尺寸，这是因为在入口处的CO含量显著增加。
经济分析显示显著节省成本，特别是节省了投资。通常，可以预期用于捕获CO2和生产CO的总投资减少5-10％。
根据本发明的一个方面，提供一种从含有二氧化碳、氢气和一氧化碳的进料气体生产至少二氧化碳和一氧化碳的方法，此方法包括至少以下步骤：
a)将进料气体压缩到高于25巴绝对的压力，
b)通过部分冷凝和/或蒸馏从已压缩的进料气体分离出至少一部分二氧化碳，从而得到二氧化碳产物和贫二氧化碳料流，
c)贫二氧化碳料流在处理单元中进行处理，从而得到含有一氧化碳和氢气的进料流，此进料流含有与贫二氧化碳料流相比更少的二氧化碳，所述进料流含有小于30摩尔％的二氧化碳，和
d)将至少一部分的含有一氧化碳和氢气的进料流加入在深冷温度下操作的分离单元，从而得到一氧化碳产物。
任选的特征包括：
-一氧化碳产物含有至少40摩尔％的一氧化碳或至少60摩尔％或至少90％的一氧化碳。
-一氧化碳产物是液态或气态的。
-一氧化碳产物可以含有至多60摩尔％的氢气或至多50摩尔％的氢气。
-二氧化碳产物是液态或气态的。
-二氧化碳产物含有至少60摩尔％的二氧化碳。
-进料气体是从生产富氢产物的变压吸附单元得到的尾气。
-分离单元得到了含氢气的料流以及进料流，并将含氢气的料流送到变压吸附单元的入口。
-进料气体是从合成气衍生的，合成气是从水蒸气甲烷重整装置、部分氧化装置或焦炭气装置得到的。
-进料气体是从合成气首先通过变换反应将一氧化碳转化成二氧化碳、然后在变压吸附单元中分离得到的。
-处理单元包括渗透单元，其用于分离贫二氧化碳料流以降低其二氧化碳含量，和用于制备含有一氧化碳和氢气的进料流或用于衍生进料流的料流。
-步骤c)包括至少两个不同的顺序排列的渗透步骤。
-第一个膜步骤的残余物通过第二个渗透步骤进行处理，并且第二个渗透单元的残余物是步骤d)中的已贫化一氧化碳的料流。
-将第一个膜步骤的渗透物循环到变压吸附单元。
-贫二氧化碳料流含有二氧化碳和一氧化碳，并且使用处理单元降低贫二氧化碳料流的一氧化碳含量，得到中间料流；并且所述处理单元还包括另一个分离步骤，其中中间料流通过吸附和/或吸收和/或渗透进行处理，从而得到含有一氧化碳和氢气的进料流以及富二氧化碳料流。
-将富二氧化碳料流送到步骤b)的分离步骤以进行分离。
-步骤d)的分离单元是部分冷凝单元、甲烷洗涤单元或一氧化碳洗涤单元。
-此方法包括在步骤d)之前将进料流的CO2含量降低到低于1％或甚至低于0.0099％。
-将CO2含量降低到低于1％或0.0099％的操作是通过吸附或胺洗涤进行的。
-此方法包括在步骤d)之前将进料流的CO2含量降低到对于在深冷温度下分离而言可接受的水平。
根据本发明的另一个方面，提供一种用于从含有二氧化碳、氢气和一氧化碳的进料气体生产至少二氧化碳和一氧化碳的设备，其包括：用于从进料气体在高于25巴绝对的压力下通过部分冷凝和/或蒸馏分离出至少一部分二氧化碳的装置，得到二氧化碳产物和贫二氧化碳料流；处理单元，其用于处理贫二氧化碳料流以得到含有一氧化碳和氢气的进料流，此进料流含有与贫二氧化碳料流相比更少的二氧化碳；分离单元，其能在深冷温度下通过蒸馏和/或汽提和/或部分冷凝进行操作；用于将至少一部分的含有一氧化碳和氢气的进料流加入分离单元的管道；和用于从分离单元取出一氧化碳产物的管道。
此设备可以另外包括：
-用于得到富氢产物的变压吸附单元，并且其中进料气体是来自变压吸附单元的尾气。
-用于从分离单元取出含氢气的料流的管道，和用于将含氢气的料流送到变压吸附单元的入口的管道。
-用于从水蒸气甲烷重整装置、部分氧化装置或焦炭气装置得到的合成气衍生进料气体的装置。
-用于从合成气衍生进料气体的装置，其包含变换反应处理单元以将一氧化碳转化成二氧化碳，并且位于变压吸附单元的上游。
-处理单元包括渗透单元，用于分离贫二氧化碳料流以降低其二氧化碳含量，并得到含有一氧化碳和氢气的进料流或用于衍生进料流的料流。
-此设备包括预处理单元，用于将进料流中的二氧化碳水平优选降低到对于随后在深冷温度下分离而言可接受的水平。
当贫二氧化碳料流含有二氧化碳和一氧化碳时，处理单元可以降低贫二氧化碳料流的一氧化碳含量，得到中间料流，并且处理单元还包括另一个分离单元，其中中间料流通过吸附和/或吸收和/或渗透进行处理，从而得到含有一氧化碳和氢气的进料流以及富二氧化碳料流。
能在深冷温度下操作的分离单元可以是部分冷凝单元、甲烷洗涤单元或一氧化碳洗涤单元。
进料气体优选作为变压吸附单元的尾气获得。这种变压吸附单元通常得到氢气作为第一产物，处于升高的压力下。
所以，整体方法按照以下顺序获得至少两种产物：
·二氧化碳
·一氧化碳。
此方法可以按照以下顺序获得三种产物：
·氢气
·二氧化碳
·一氧化碳。
下面将参考显示本发明工艺的附图更详细地描述本发明方法。
在图1中，将天然气GN加入合成气产生器R的燃烧器，从而处理含有氢气、一氧化碳和二氧化碳的合成气1。在变换转化之后，变换气体3在PSA单元中分离以得到富氢产物，以及含有二氧化碳、一氧化碳和氢气的残余气体5，气体5的氢气含量小于气体3的氢气含量。
将残余气体5压缩到高于25巴绝对的压力，并在CPU中在低于环境温度的温度下通过部分冷凝和/或蒸馏进行分离，得到二氧化碳产物和贫二氧化碳料流。贫二氧化碳料流7在处理单元T中进行处理，得到进料流15，其主要含有一氧化碳和氢气以及优选含有小于1％或甚至小于0.0099％的二氧化碳。将料流15送到在深冷温度下通过部分冷凝和/或蒸馏操作的分离单元HYCO，得到含有至少40％一氧化碳、至少60％一氧化碳或至少90％一氧化碳的料流。此料流可以例如含有至少40％的一氧化碳和小于60％的氢气。
处理单元T也可以获得料流21和/或料流9，它们含有二氧化碳，优选含有至少二氧化碳。
在图中，将料流21送到PSA单元的上游，和将料流9送到CPU单元的上游。
分离单元HYCO也可以得到含有甲烷的料流19，其被送回合成气产生器，作为燃料。分离单元HYCO也可以得到富含氢气的料流17，其含有至少50％的氢气。将此料流送到氢气PSA的上游。
为了说明处理单元7的内容，图2显示其中单元T由位于吸收单元MDEA上游的渗透单元M组成的情况，其中进行胺洗涤操作。
在这里，贫二氧化碳料流7用渗透单元M分离以形成料流11，其中仍然进一步减少二氧化碳并且富集甲烷和一氧化碳。
将料流11送到胺洗涤MDEA以生产进料流15，其主要含有甲烷、氢气和一氧化碳。
进料流15在深冷分离单元HYCO中分离，例如通过部分冷凝工艺进行分离。也可以采用甲烷洗涤工艺或一氧化碳洗涤工艺。
这得到了：富含一氧化碳的料流，其含有至少40％的一氧化碳；富含甲烷的料流19，其作为燃料被送回合成气产生器；以及富含氢气的料流17，其被送到PSA单元的上游。
通过胺洗涤得到的富二氧化碳料流13被送回CPU。
下表显示了图2所示料流的摩尔百分比纯度。

Claims (12)

1.一种从含有二氧化碳、氢气和一氧化碳的进料气体生产至少二氧化碳和一氧化碳的方法，此方法包括至少以下步骤：
a)将进料气体(5)压缩到高于25巴绝对的压力，其中进料气体(5)是来自用于生产富氢产物的变压吸附单元(PSA)的尾气，并且变压吸附单元的进料是来自合成气产生器(R)，
b)通过部分冷凝和/或蒸馏从已压缩的进料气体分离出至少一部分二氧化碳，得到二氧化碳产物和贫二氧化碳料流(7)，
c)贫二氧化碳料流在处理单元(S)中进行处理，从而得到含有一氧化碳、甲烷和氢气的进料流(15)，此进料流含有与贫二氧化碳料流相比更少的二氧化碳，所述进料流含有至少30摩尔％的一氧化碳，和
d)将至少一部分的含有一氧化碳、甲烷和氢气的进料流加入在深冷温度下操作的分离单元(HYCO)，得到含有至少40摩尔％一氧化碳的一氧化碳产物，并且分离单元得到含有甲烷的料流(19)，此料流作为燃料被送回合成气产生器；并且分离单元得到富含氢气的料流(17)，其含有至少50％的氢气，此料流被送到变压吸附单元的上游。
2.根据权利要求1的方法，其中进料气体是衍生自合成气(1)，合成气是从水蒸气甲烷重整装置、部分氧化装置或焦炭气装置得到的。
3.根据权利要求1或2的方法，其中进料气体(5)是从合成气(1)首先通过变换反应以将一氧化碳转化成二氧化碳、然后在变压吸附单元(PSA)中分离得到的。
4.根据权利要求1或2的方法，其中处理单元(S)包括渗透单元(M)，其用于分离贫二氧化碳料流以降低其二氧化碳含量，并得到含有一氧化碳、甲烷和氢气的进料流(15)或用于衍生进料流的料流(11)。
5.根据权利要求4的方法，其中步骤c)包括至少两个不同的顺序排列的渗透步骤。
6.根据权利要求5的方法，其中步骤c)包括两个不同的渗透步骤，其中第一个渗透步骤的残余物通过第二个渗透步骤进行处理，并且第二个渗透单元的残余物是步骤d)中的已贫化一氧化碳的料流。
7.根据权利要求1或5的方法，其中步骤c)包括两个不同的渗透步骤，将第一个渗透步骤的渗透物(21)循环到变压吸附单元(PSA)。
8.根据权利要求1或2的方法，其中贫二氧化碳料流含有二氧化碳和一氧化碳，并且使用处理单元(S)降低贫二氧化碳料流的一氧化碳含量，得到中间料流(11)；并且所述处理单元还包括另一个分离步骤，其中中间料流通过吸附和/或吸收和/或渗透进行处理，从而得到含有一氧化碳、甲烷和氢气的进料流(15)以及富二氧化碳料流(13)。
9.根据权利要求8的方法，其中进料流(15)含有低于1％的二氧化碳或甚至低于0.0099％的二氧化碳。
10.根据权利要求8的方法，其中将富二氧化碳料流(13)送到步骤b)的分离步骤(CPU)以进行分离。
11.根据权利要求1或2的方法，其中步骤d)的分离单元(HYCO)是部分冷凝单元、甲烷洗涤单元或一氧化碳洗涤单元。
12.一种用于从含有二氧化碳、氢气和一氧化碳的进料气体生产至少二氧化碳和一氧化碳的设备，其包括：
变压吸附单元(PSA)，其能得到含有二氧化碳、氢气和一氧化碳的尾气以及富氢产物；
用于将合成气从合成气产生器作为进料送到变压吸附单元的装置；
用于将尾气压缩到高于25巴绝对的压力的压缩装置；
装置(CPU)，其用于从经压缩的尾气在高于25巴绝对的压力下通过部分冷凝和/或蒸馏分离出至少一部分的二氧化碳，得到二氧化碳产物和贫二氧化碳料流；
处理单元(S，M，MDEA)，其用于处理贫二氧化碳料流以得到含有一氧化碳、甲烷和氢气的进料流(15)，此进料流含有与贫二氧化碳料流相比更少的二氧化碳；
分离单元(HYCO)，其能在深冷温度下通过蒸馏和/或汽提和/或部分冷凝进行操作；
用于将至少一部分的含有一氧化碳、甲烷和氢气的进料流加入分离单元的管道；
用于从分离单元取出含有至少50％氢气的富含氢气的料流的管道；
用于从分离单元取出一氧化碳产物的管道；
与变压吸附单元上游处连接的用于从分离单元取出富含氢气的料流的管道；和
与合成气产生器入口连接的用于从分离单元取出作为燃料的含甲烷的料流(19)的管道。
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