CN116710397A - 利用与变压吸附单元和/或低温分离系统集成的气体分离膜提高氢气回收 - Google Patents

利用与变压吸附单元和/或低温分离系统集成的气体分离膜提高氢气回收 Download PDF

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CN116710397A
CN116710397A CN202280009222.2A CN202280009222A CN116710397A CN 116710397 A CN116710397 A CN 116710397A CN 202280009222 A CN202280009222 A CN 202280009222A CN 116710397 A CN116710397 A CN 116710397A
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stream
swing adsorption
tail gas
pressure swing
hydrogen
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谢卡尔·特瓦里
罗纳德·M·文纳
苏尼尔·潘迪拉奥
丹尼斯·马洛尼
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CB&I Technology Inc
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Lummus Technology Inc
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Abstract

用于回收氢气的方法和系统可以包括将包含氢气和附加气体的气体物流进给至变压吸附(PSA)系统，并将包含氢气的膜渗透物流进给至PSA系统。在PSA系统中，可以将氢气的一部分与附加气体分离，以回收氢气产物物流以及包含未分离的氢气和附加气体的PSA尾气物流。可以将PSA尾气物流进给至膜分离单元，用于将氢气与附加气体分离，并回收(i)进给至PSA系统的包含氢气的膜渗透物流和(ii)包含附加气体的膜尾气物流。本文的实施方案还可以包括用于部分冷凝进料气体物流和PSA尾气物流中的一者或两者的制冷系统，从而提高膜分离单元的效率。

Description

利用与变压吸附单元和/或低温分离系统集成的气体分离膜 提高氢气回收
技术领域
本发明的实施方案一般地涉及从气体物流中回收氢气。
背景技术
许多石油化工工艺使用或产生氢气(H2)，并且未反应的或产生的氢气通常被回收以供在石油化工工厂内再循环或使用。目前，通常使用变压吸附(PSA)单元或低温分离单元从混合气体物流中回收氢气，而产生的尾气被发送至燃料气体池。
PSA和低温分离具有能够回收的最大H2量的技术限制。总会有一些氢气在尾气物流中损失掉。这些配置的主要缺点是将氢气损失到低价值物流中，导致单元的整体运营费用较高。
发明内容
本文的实施方案将气体分离膜与PSA和/或低温分离相集成，以提高氢气的整体回收率，并最大限度地减少高价值氢气向低价值燃料气体物流的损失。这种附加的氢气回收可以提供节省运营费用的显著益处。这也将二氧化碳(CO2)浓缩在产生的尾气中，这使得尾气物流中的碳捕获更加高效和经济。
在一方面，本文公开的实施方案涉及用于回收氢气的方法。用于回收氢气的方法可以包括将包含氢气和附加气体的气体物流进给至变压吸附(PSA)系统，并将包含氢气的膜渗透物流进给至PSA系统。在PSA系统中，可以将氢气的一部分与附加气体分离，以回收氢气产物物流以及包含未分离的氢气和附加气体的PSA尾气物流。可以将PSA尾气物流进给至膜分离单元，用于将氢气与附加气体分离，以回收(i)进给至PSA系统的包含氢气的膜渗透物流和(ii)包含附加气体的膜尾气物流。
在一些实施方案中，该方法还可以包括在膜分离单元的上游压缩变压吸附尾气物流。在一些实施方案中，该方法还可以包括在变压吸附系统的上游压缩膜渗透物流。本文的方法的实施方案还可以包括部分冷凝进料气体物流和PSA尾气物流中的一者或两者。
在另一个方面，本文公开的实施方案涉及用于回收氢气的系统。该系统可以包括用于将包含氢气和附加气体的气体物流进给至变压吸附系统的流动管线，和用于将包含氢气的膜渗透物流进给至变压吸附系统的流动管线。该系统还包括变压吸附系统，该变压吸附系统可以被配置为将氢气的一部分与附加气体分离，以回收氢气产物物流以及包含未分离的氢气和附加气体的变压吸附尾气物流。可以提供流动管线，用于将变压吸附尾气物流进给至膜分离单元，该膜分离单元可以被配置为将氢气与附加气体分离，并回收(i)进给至变压吸附系统的包含氢气的膜渗透物流和(ii)包含附加气体的膜尾气物流。
在一些实施方案中，该系统还可以包括用于在膜分离单元的上游压缩变压吸附尾气物流的压缩机。在一些实施方案中，该系统还可以包括用于在变压吸附系统的上游压缩膜渗透物流的压缩机。本文的系统的实施方案还可以包括用于部分冷凝进料气体物流和PSA尾气物流中的一者或者两者的制冷/分离系统。
其他方面和优点将从以下的描述和所附的权利要求中变得清楚。
附图说明
图1是典型的变压吸附系统的简化工艺流程图。
图2和图3是根据本文公开的一个或多个实施方案的用于回收氢气的集成系统的简化工艺流程图。
具体实施方式
本文的实施方案尤其涉及从来自石油化工工艺的混合气体物流(诸如，工艺气体、废气体、散发气体或尾气物流)中回收氢气。例如，进给的用于氢气回收的混合气体物流可以包括氢气、二氧化碳、一氧化碳、硫化氢、硫氧化物、氮气、氧气、甲烷、乙烷、乙烯和/或丙烷以及其他组分。虽然注意到了石油化工物流，但是本文所描述的实施方案可以用于期望从其中回收氢气的任何含氢气的气体物流。
现有技术利用独立的PSA单元从工艺气体或废气体物流中回收H2。本文的实施方案将PSA与膜系统集成在一起，或将PSA和低温分离系统与膜系统集成在一起，以提高H2的整体回收率。因此，本文的实施方案在氢气回收参数和回收块的配置方面不同于现有技术。
本文的实施方案可以利用膜和PSA将本文所描述的系统定位在气体物流上，以回收通常损失于尾气物流中的H2。来自膜的渗透物可以再循环回PSA用于H2的附加回收。在一些实施方案中，可以利用低温分离来改善膜系统的进料质量。
图1中示出了典型的现有技术PSA系统的简单方块流程图。工艺气体或废气体物流10可以是目标用于H2回收的任何气体物流，该工艺气体或废气体物流10可以在适当的压力下进给至PSA单元12以回收氢气产物14。剩余气体(包括任何未回收的H2)作为尾气物流16被发送，尾气物流16通常在单元中用作燃料气体。如上所述，从PSA单元中整体回收氢气会导致氢气大量损失于尾气物流16中。PSA单元通常可以回收进料物流中85至90％的氢气，而余量的氢气永久损失于尾气中。
本文的实施方案可以通过在回收系统内适当地并入膜分离来增强尾气物流中H2的回收。尾气可以在适当的压力下进给至膜分离单元。如有必要，可以使用压缩机对膜系统所需的气体加压，以实现目标H2回收率和纯度。然后，可以将来自膜的富含氢气的渗透物流再循环回PSA单元，用于附加回收H2于最终的PSA产物中，而渗余物流可以从联合单元中回收作为尾气物流，并可以用作燃料气体物流，发送至碳捕获，或用于一些其他目的。
现在参考图2，图示了根据本文的实施方案的用于回收氢气的系统的简化工艺流程图。工艺气体或废气体物流1、2可以是目标用于H2回收的任何气体物流，该工艺气体或废气体物流1、2可以在适当的压力(诸如25至35barg)下进给至PSA单元22，用于回收氢气产物3和剩余气体4。
物流4中的剩余气体(包括任何未回收的H2)可以通过流动物流4发送至膜分离系统24。如果需要，可以使用压缩机26来增加物流4中剩余气体的压力，产生经加压的剩余气体物流5，其可以进给至膜分离系统24。例如，剩余气体可以在1至5barg范围内的压力下回收于物流4中，并且剩余气体的压力可以增加至在10至20barg范围内的压力，然后通过流动物流5进给至膜分离系统24。
在膜分离系统24中，膜用于将氢气与剩余气体物流4、5中的其他气体分离。氢气渗透物可以通过流动物流7回收，而渗余物流(未渗透通过膜的气体)可以回收作为尾气物流6。然后，可以将氢气渗透物7再循环至变压吸附单元22，用于与进料物流1一起回收氢气。如果需要，可以使用压缩机28来增加渗透物流7中氢气的压力，产生经加压的渗透物流8，其可以进给至PSA单元22。例如，富含氢气的渗透物流7可以在1至2barg范围内的压力下从膜分离系统24中回收，并且可以再循环回PSA单元，用于附加回收氢气于最终的产物中。渗余物流(即尾气物流6)可以在较高的压力(诸如，在8至18barg的范围内)下回收，并且来自联合单元的该尾气物流可以用作燃料气体物流，被发送用于碳捕获，或者用作一些其他目的的气体。
虽然可以使用主要回收渗透物中的H2的膜，但是一些其他气体也可以与H2一起回收于渗透物流7中。这些气体将在系统中达到稳态浓度，并最终在PSA单元中除去，并最终通过尾气物流6离开系统。
膜分离系统24可以回收PSA尾气4中的70％至90％的氢气，从而从类似于图2所描绘的系统中得到在96％至99％范围内的整体氢气回收率。
在一些实施方案中，工艺气体或废气体可以包括可冷凝组分，诸如轻质烃类(甲烷、乙烷等)或其他较重质的气体。在一些这样的实施方案中，可以对来自PSA单元的尾气物流进行低温分离，以冷凝较重质的烃类，而轻馏分可以在膜系统中处理。在膜单元中处理较高纯度的H2气体物流可以提供更好的H2回收率和纯度。较高纯度H2的好处还可以用于在较低压力下操作膜系统，同时实现类似于在没有冷却器的配置中实现的氢气回收率。低温分离还可以有益地降低可能影响膜性能或与膜材料不相容的组分的浓度。
现在参考图3，图示了根据本文的实施方案的将低温分离、PSA和膜分离集成用于回收氢气的系统的简化工艺流程图，其中相同的数字表示相同的部件。
类似于图2的实施方案，工艺气体或废气体物流1、2可以是目标用于H2回收的任何气体物流，该工艺气体或废气体物流1、2可以在适当的压力下进给至PSA单元22，以回收氢气产物3。剩余的气体(包括任何未回收的H2)可以通过流动物流4发送至膜分离系统24。在膜分离系统24中，膜用于将氢气与剩余气体物流4中的其他气体分离。氢气渗透物可以通过流动物流7回收，而渗余物流(未渗透通过膜的气体)可以回收作为尾气物流6。然后，可以将氢气渗透物7与工艺气体或废气体物流1组合，并通过流动管线2再循环至变压吸附单元22，用于回收氢气。
为了增强PSA单元22和膜分离系统24中的每一个中的分离，可以使用低温分离系统31。可以在冷却器33中冷却进料物流32，诸如包括氢气和可冷凝组分(诸如轻质烃类)的贫含工艺气体或废气体物流，从而降低气体物流32的温度并冷凝可冷凝组分的一部分。可以将所得的经冷却的进料物流35进给至蒸气-液体分离器37，诸如闪蒸罐、蒸馏塔等，以将任何冷凝组分与蒸气分离。冷凝组分可以回收作为塔底液体物流39，而未冷凝的蒸气可以回收作为塔顶物流41。然后，塔顶物流41可以通过冷却器33，产生进给至PSA单元22的工艺气体物流或废气体物流1。
除了未回收的氢气之外，PSA尾气物流4还可以含有可冷凝组分，诸如在蒸气-液体分离器37中未冷凝和回收的任何轻质烃类。可以冷却PSA尾气物流4以冷凝可冷凝组分的至少一部分，并将其进给至第二蒸气-液体分离器43，以回收第二塔顶物流49和第二塔底物流50。
例如，可以使用冷却器33和/或第二冷却器45中的交叉交换来进行PSA尾气物流的冷却。在一些实施方案中，PSA尾气物流最初通过冷却器33进行处理，然后通过物流47进给至冷却器45，并与第二蒸气-液体分离器43塔顶物流49进行交叉交换。在交叉交换之后，可以将冷冻了的PSA尾气物流51进给至第二蒸气-液体分离器43，用于将冷凝组分与未冷凝的PSA尾气组分分离，冷凝组分通过流动管线50回收，未冷凝的PSA尾气组分通过塔顶物流49回收。
在冷却器45和/或冷却器33中的交叉交换之后，塔顶物流49(未冷凝的PSA尾气)可以通过流动物流55进给至膜分离单元24，并如上文所描述的进行处理。通过流动管线39、50从分离器37、43回收的冷凝组分可以合并，形成合并的冷凝物流57。合并的冷凝物流57可以膨胀或以其他方式用于冷却器33中的交叉交换，并回收作为燃料气体产物物流59。
虽然未在图3中图示，但冷却器33、45中的一者或两者可以包括制冷剂进料物流，以提供所期望的物流的所期望的制冷和冷却。附加地或替代地，可以将各种物流压缩和/或膨胀，以在冷却器33、45内提供期望的制冷量，从而导致部分冷凝。
作为实施例，使用适当的制冷剂(诸如，丙烯和/或乙烯或由制冷剂物流或工艺物流提供的制冷的任何组合)在冷却器33中将在20至30barg的压力下的贫含工艺气体物流32冷冻至-37℃至-60℃的温度。然后，可以将经冷却的进料物流35在20至30barg的压力下操作的蒸气-液体分离器37中闪蒸。将来自分离器的蒸气41加热回在35至45℃范围内的温度，然后将其通过流动物流1、2送至PSA单元22以回收氢气产物物流3。
将来自PSA单元22的剩余气体4在使用甲烷/丙烯/乙烯或任何组合制冷的一系列冷却器中进一步冷却至在-60℃至-98℃范围内的温度。例如，剩余气体4可以最初在交换器33中冷却，并在交换器45中进一步冷却，产生经冷却的剩余气体物流51。然后，剩余气体物流51可以在蒸气-液体分离器43中闪蒸。将来自分离器43的蒸气在交叉交换器/冷却器45、33中加热回35至45℃的温度，然后通过流动管线55送至膜分离单元24。然后，将来自膜分离单元24的富含氢气的渗透物7进行压缩并再循环回PSA单元22用于附加氢气回收，而将渗余物6作为系统尾气送至燃料气总管。
虽然图3图示了两个交叉交换器33、45和两个蒸气-液体分离器37、43，但根据提纯来自PSA单元的剩余气体4中的H2的需要或基于将进料55中的H2浓缩至膜分离单元24的需要，可以使用更低温度下的附加交换器和分离器。
根据本文的实施方案，PSA、低温分离和膜的组合可以提供在96至99％范围内的整体H2回收率。
集成诸如在图3的实施方案中的低温分离可以冷凝较重质的烃类，而可以在膜系统中处理轻馏分(包括工艺气体或废气体中存在的氢气和其他不可冷凝的组分)。这可以导致在膜单元中处理具有较高纯度的进料气体物流，这可以提供较好的H2回收率和纯度。较高纯度H2的益处也可以用于在较低压力下操作膜系统。
对于所有这些配置，膜系统可以是单级或多级系统，这取决于膜渗透物中H2纯度和H2回收率的要求。穿过膜的H2纯度和回收率影响穿过膜集成PSA系统的H2的整体回收率。
本文的实施方案还可以扩展至H2回收方法的其他模式。还通过低温分离回收H2，其中制冷剂用于回收H2。在这样的实施方案中，膜可以用于提高H2的回收率，从而降低制冷系统的负荷，导致该方法的经济性更好。
如上所述，通过图2和图3中所图示的方法产生的尾气体物流7可以用作燃料气体或用于一些其他工艺气体。任选地，可以将含有一氧化碳、二氧化碳或其他含碳分子的尾气体物流进给至碳捕获单元。由本文所描述的方法得到的较高的氢气回收率可以导致较少量的尾气进入下游碳捕获单元。此外，较低的氢气量或几乎没有氢气，也有助于将进料中的二氧化碳浓缩至碳捕获单元，从而产生更高效的脱碳。较低的氢气浓度和数量也可以导致碳捕获单元所需的工艺单元大小较小，从而降低这些单元的资本成本。
如上所述，本文的实施方案利用PSA和/或低温分离与膜分离以改善从混合气体物流中的氢气回收。改善的氢气回收通过避免高价值氢气损失于低价值燃料气体池中，而提供节省相关联设备的运营费用的益处。此外，这也将有助于使尾气脱碳(从尾气中捕获碳)更高效，容量更小。
除非另有定义，否则所使用的所有技术和科学术语具有与这些系统、装置、方法、工艺和组合物所属领域的普通技术人员通常理解的含义相同的含义。
单数形式“一个/种(a)”、“一个/种(an)”和“该/所述(the)”包括复数指示物，除非上下文另有明确规定。
如这里和所附权利要求中所用的，词语“包括”、“具有”和“包含”及其所有语法变体均旨在具有不排除附加元素或步骤的开放的、非限制性的含义。
“任选地”是指随后描述的事项或情况可以发生或可以不发生。描述包括事项或情况发生的实例和事项或情况不发生的实例。
当使用词语“大约”或“约”时，该术语可能意味着值的变化可以至多±10％、至多5％、至多2％、至多1％、至多0.5％、至多0.1％或至多0.01％。
范围可以表示为从约一个特定值至约另一个特定值，包括端点值。当表达这样的范围时，应当理解的是，另一个实施方案是从一个特定值到另一个特定值，以及该范围内的所有特定值及其组合。
虽然本公开包括有限数量的实施方案，但受益于本公开的本领域技术人员将理解，可以设计不脱离本公开的范围的其他实施方案。因此，其范围应仅受所附权利要求的限制。

Claims (16)

1.一种用于回收氢气的方法，所述方法包括：
将包含氢气和附加气体的气体物流进给至变压吸附系统；
将包含氢气的膜渗透物流进给至所述变压吸附系统；
在所述变压吸附系统中，将所述氢气的一部分与所述附加气体分离，以回收氢气产物物流以及包含未分离的氢气和所述附加气体的变压吸附尾气物流；
将所述变压吸附尾气物流进给至膜分离单元；和
在所述膜分离单元中，将氢气与所述附加气体分离，以回收(i)进给至所述变压吸附系统的包含氢气的所述膜渗透物流和(ii)包含所述附加气体的膜尾气物流。
2.根据权利要求1所述的方法，还包括在所述膜分离单元的上游压缩所述变压吸附尾气物流。
3.根据权利要求1或权利要求2所述的方法，还包括在所述变压吸附系统的上游压缩所述膜渗透物流。
4.根据权利要求1至3中任一项所述的方法，还包括部分冷凝所述气体物流，回收冷凝物流和蒸气物流，以及将所述蒸气物流作为进给至所述变压吸附系统的所述气体物流进给。
5.根据权利要求1至4中任一项所述的方法，还包括部分冷凝所述变压吸附尾气物流，回收PSA尾气冷凝物流和PSA尾气蒸气物流，并将所述PSA尾气蒸气物流作为进给至所述膜分离单元的所述变压吸附尾气物流进给。
6.根据权利要求1至5中任一项所述的方法，其中将所述气体物流在25至35barg范围内的压力下进给至所述变压吸附系统。
7.根据权利要求1至6中任一项所述的方法，其中所述变压吸附尾气物流在1至5barg范围内的压力下从所述变压吸附系统中回收，并在被进给至所述膜分离单元之前被压缩至10至20barg的压力。
8.根据权利要求1至7中任一项所述的方法，其中所述膜渗透物流在1至2barg范围内的压力下从所述膜分离单元中回收，并被压缩至25至35barg范围内的压力，用于进给至所述变压吸附系统。
9.根据权利要求1至8中任一项所述的方法，其中所述膜尾气物流在8至18barg范围内的压力下回收。
10.一种用于回收氢气的系统，所述系统包括：
用于将包含氢气和附加气体的气体物流进给至变压吸附系统的流动管线；
用于将包含氢气的膜渗透物流进给至所述变压吸附系统的流动管线；
所述变压吸附系统，被配置为将所述氢气的一部分与所述附加气体分离，以回收氢气产物物流以及包含未分离的氢气和所述附加气体的变压吸附尾气物流；
用于将所述变压吸附尾气物流进给至膜分离单元的流动管线；和
所述膜分离单元，被配置为将氢气与所述附加气体分离，并回收(i)进给至所述变压吸附系统的包含氢气的所述膜渗透物流和(ii)包含所述附加气体的膜尾气物流。
11.根据权利要求10所述的系统，还包括用于在所述膜分离单元的上游压缩所述变压吸附尾气物流的压缩机。
12.根据权利要求10或权利要求11所述的系统，还包括用于在所述变压吸附系统的上游压缩所述膜渗透物流的压缩机。
13.根据权利要求10至12中任一项所述的系统，还包括用于部分冷凝所述气体物流、回收冷凝物流和蒸气物流的制冷/分离系统，以及用于将所述蒸气物流作为进给至所述变压吸附系统的所述气体物流进给的流动管线。
14.根据权利要求10至12中任一项所述的系统，还包括制冷/分离系统，所述制冷/分离系统被配置为部分冷凝所述变压吸附尾气物流，回收PSA尾气冷凝物流和PSA尾气蒸气物流，并且将所述PSA尾气蒸气物流作为进给至所述膜分离单元的所述变压吸附尾气物流进给。
15.根据权利要求10至12中任一项所述的系统，还包括制冷/分离系统，所述制冷/分离系统被配置为：
部分冷凝所述气体物流，回收冷凝物流和蒸气物流，以及用于将所述蒸气物流作为进给至所述变压吸附系统的所述气体物流进给的流动管线；和
部分冷凝所述变压吸附尾气物流，回收PSA尾气冷凝物流和PSA尾气蒸气物流，并将所述PSA尾气蒸气物流作为进给至所述膜分离单元的所述变压吸附尾气物流进给。
16.根据权利要求15所述的系统，其中所述制冷/分离系统包括：
被配置为在所述气体物流、所述变压吸附尾气物流、所述蒸气物流、所述PSA尾气蒸气物流、所述冷凝物流和所述PSA尾气冷凝物流的混合物和制冷剂之间交换热量的交叉交换器，产生部分冷凝的气体物流；
被配置为在所述变压吸附尾气物流和所述PSA尾气蒸气物流之间交换热量的交叉交换器，产生部分冷凝的变压吸附尾气物流；
蒸气-液体分离器，所述蒸气-液体分离器被配置为接收所述部分冷凝的气体物流，所述蒸气-液体分离器包括用于回收所述蒸气物流的蒸气出口和用于回收所述冷凝物流的液体出口；和
第二蒸气-液体分离器，所述第二蒸气-液体分离器被配置为接收所述部分冷凝的变压吸附尾气物流，所述第二蒸气-液体分离器包括用于回收所述PSA尾气蒸气物流的蒸气出口和用于回收所述PSA尾气冷凝物流的液体出口。
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