CN116507870A - 生产液化氢的方法 - Google Patents

生产液化氢的方法 Download PDF

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CN116507870A
CN116507870A CN202180074434.4A CN202180074434A CN116507870A CN 116507870 A CN116507870 A CN 116507870A CN 202180074434 A CN202180074434 A CN 202180074434A CN 116507870 A CN116507870 A CN 116507870A
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stream
hydrogen
bar
heat exchanger
outlet
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杰弗里·弗雷德里克·斯金纳
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Gasconsult Ltd
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Abstract

用于液化氢气的工艺包括：通过与在设置有高温膨胀器和低温膨胀器的制冷回路中循环的制冷剂进行热交换，将氢气冷却至中间温度，来自低温膨胀器的出口流含有一些冷凝制冷剂；提供从循环制冷剂中分离冷凝物的装置；通过与冷凝物的蒸发和再加热进行热交换来进一步冷却氢气。制冷回路中的流体通常是甲烷(诸如去除二氧化碳、水蒸气和其他杂质后的天然气)、氮，或其混合物。

Description

生产液化氢的方法
技术领域
本发明涉及一种用于液化氢气的方法，特别是一种在液化之前将待液化的氢冷却至中间温度的方法。
背景技术
液化氢是含碳燃料的潜在替代品。除了目前在太空应用中的用途外，未来还需要大量的液态氢作为航空和航运的燃料。随着氢作为燃料的使用增加，对以液体形式的氢的大规模储存和运输的需求将会发展。
现有的和提出的氢液化工艺主要包括：
-通过与蒸发流体(“第一制冷剂”)的热交换将进入的氢冷却(在下文中称为“预冷却”)至中间温度(在下文中称为“中间温度”)的第一步骤；最广泛建议的第一制冷剂流体是液态氮和液态甲烷(LNG)，并且还建议混合制冷剂，以及
-通过部分预冷却氢或第二制冷剂(诸如氦)的功膨胀进一步冷却和液化预冷却氢的第二步骤。
尽管不进行任何预冷却并且仅包括前述第二步骤(通过氢或第二制冷剂的膨胀的制冷)的氢液化工艺是可行的并且可能已经实践过，但由于两个因素：(a)整个液化工艺的总压缩功率的降低，以及(b)由于第二制冷剂系统的循环速率和压缩功率的降低而导致的可感知的较低的投资和生产成本，因此优选地是加入预冷却的第一步骤。
关于因素(b)，在第一预冷却步骤的出口处使用氢的最低实际温度(通常使用液态氮作为第一制冷剂时未为-190℃左右)将使所需的循环速率最小化，从而使第二步骤中的制冷剂的压缩功率最小化。然而，当考虑到预冷却系统的压缩功率需求时，最低实际预冷却温度不一定会导致整个液化工艺的最低总压缩功率。
发明内容
本发明的主要方面涉及氢的液化，并且公开了将待液化的氢流预冷却至通常介于-150℃至-200℃之间的中间温度的改进方法。
压力在本申请中以“巴”表示，这些压力是巴的绝对值。
所公开的预冷却装置是包含流体(诸如但不限于甲烷或氮或其混合物)的封闭循环，该封闭循环包括：
-高温气体膨胀器机器，该高温气体膨胀器机器具有气体出口流；
-低温气体膨胀器机器，该低温气体膨胀器机器具有部分液化的出口流；
-从低温气体膨胀器机器的出口流中分离液体；
-将分离的液体减压至接近大气压力；
-从接近环境温度连续冷却进料氢(以及第二制冷剂，如果使用的话)，首先通过与来自所述高温气体膨胀器的出口流进行热交换；其次通过在液体分离后与来自所述低温气体膨胀器的出口流进行热交换；最后通过与减压的所述液态制冷剂的蒸发进行热交换而达到-150℃至-200℃的典型中间温度；
-将得到的低压制冷剂流进行再压缩。
上述预冷却循环的布置，特别是在低温气体膨胀器中形成液体，随后将液体从低温气体膨胀器出口流中分离类似于GB2486036中描述的用于甲烷液化(LNG生产)的工艺。虽然在该参考情况下，在低温气体膨胀器中形成的液体贡献了该工艺的总液体(LNG)输出的一部分，但在该申请中，液体被减压，然后通过热交换器与待液化的氢一起蒸发，以在氢液化过程中将氢冷却到通常为-150℃至-200℃的中间温度。
本发明包括在高温气体膨胀器机器中使用甲烷作为制冷剂，而在低温气体膨胀器机器中使用氮作为制冷剂。
申请人认为，该冷却待液化的氢的方法(即在气体膨胀器中形成液体制冷剂，将液体分离、减压以及蒸发作为氢液化过程中的预冷却剂)在现有技术中尚未公开，并且是新颖的。液体的产生是热效率的，因为液体是由低温气体膨胀器中的机械功直接产生的。在氢液化过程中产生液态制冷剂(诸如液态甲烷或液态氮)也有实际好处，消除了对昂贵且精细的液态第一制冷剂(诸如混合制冷剂)的外部供应的需求。
因此，以下提供了根据本发明的主要方面的用于液化氢的工艺的说明(参照图1/3(图1)以及图上所示的设备标签和流编号)：
-提供纯氢进料气体流[1]；
-以1巴至50巴的压力提供再循环氢气流[2]；
-使流[1]和[2]进入氢压缩机[A]，所述压缩机具有冷却后的合并排放流[3]，该合并排放流的压力介于10巴至200巴之间，更典型地，压力介于20巴至100巴之间；
-在热交换器[B]的第一热通道中冷却所述合并排放流[3]，所述热通道具有出口流[4]；
-在热交换器[C]的第一热通道中冷却所述流[4]，所述热通道具有出口流[5]；
-在热交换器[D]的第一热通道中冷却所述流[5]，所述热通道具有出口流[6]；
-使流[6]进入氢液化单元[E]；
-氢液化单元[E]通常包括：将流[6]分成两部分；在第一气体膨胀器中冷却第一部分[e-1]以形成出口流[e-2]；在第一热交换器中冷却第二部分[e-3]以形成流[e-4]；将流[e-4]分成两部分；在第二气体膨胀器中冷却第一部分[e-5]以形成出口流[e-6]；在第二热交换器中冷却和液化第二部分[e-7]以形成液化氢生成物流[7]；通过第二热交换器再循环流[e-6]以形成流[e-8]；合并流[e-2]和[e-8]以形成流[e-9]；在第一热交换器中再加热流[e-9]以形成再循环氢流[8]；在第二热交换器中提供催化剂以促进邻位氢向对位氢的转化；
-液化氢生成物流[7]的温度介于-240℃至-255℃之间；
-再循环氢流[8]的压力介于1巴和30巴之间；在热交换器[D]的第一冷通道中再加热流[8]，形成出口流[9]；在热交换器[C]的第一冷通道中再加热流[9]，形成出口流[10]；在热交换器[B]的第一冷通道中再加热流[10]，来自热交换器[B]的被再加热的流形成上述氢再循环气体流[2]；
-热交换器[B]、[C]和[D]可以被物理地结合在单个单元中；
-提供压力为10巴至150巴的制冷剂气体流[21]；
-将制冷剂气体流[21]分成第一部分[22]和第二部分[25]；
-使所述第一部分[22]进入第一制冷剂气体膨胀器[L]，来自所述第一制冷剂气体膨胀器的出口流[23]具有介于5巴至50巴之间的压力；
-在热交换器[B]的第二冷通道中再加热第一制冷剂气体膨胀器出口流[23]以形成再加热流[24]；
-在压缩机[M]中将被再加热的流[24]压缩到10巴至150巴的压力，以在冷却后形成上述制冷剂气体[21]的第一组分；
-使制冷剂气体的第二部分[25]进入热交换器[B]的第二热通道，该第二热通道具有出口流[26]；
-使冷却的所述制冷剂气体的第二部分[26]进入第二制冷剂气体膨胀器[N]，来自所述第二制冷剂气体膨胀器的出口流[27]具有通常介于3巴至50巴之间的压力，并且包括蒸汽和液体的混合物；
-在蒸汽/液体分离器[O]中分离第二气体膨胀器[N]的出口流[27]，以形成蒸汽流[28]和液体流[29]；
-通常在阀[P]中将所述液体流[29]进行减压，以形成压力介于0.5巴至10巴之间并且通常处于接近大气压力的流[30]；流[30]的温度通常为-160℃(以甲烷作为制冷剂)和-195℃(以氮作为制冷剂)，两者都基本处于大气压力下；
-在热交换器(D)的第二冷通道中蒸发和再加热流[30]，以形成出口蒸汽流[31]；
-通过具有出口流[32]的制冷剂压缩机[Q]将流[31]压缩至与流[28]的压力相同的压力；
-合并流[28]和流[32]以形成流[34]；
-在热交换器[C]的第二冷通道中再加热流[34]以形成流[35]，然后在热交换器[B]的第三冷通道中再加热流以形成流[36]；
-在压缩机[M]中将被再加热的流[36]压缩至10巴至150巴的压力，以在冷却后形成上述制冷剂气体[21]的第二组分。
本发明的第二方面是利用上述二级膨胀器预冷却回路的高效率，以明显低于环境的吸入温度运行氢再循环压缩机。建议的流程示意图如图2/3(图2)所示。流[9]通常以-120℃的温度进入压缩机A的第一部分。
替代性地，压缩机[A]的入口流可以直接从氢液化器单元[E]的出口流[8]获得，或者从图1/3(图1)上的热交换器[C]的第一冷通道[10]的出口获得；
根据压缩机[A]的入口温度，相对于图1/3(图1)所示的具有环境入口温度的构型，所述压缩机[A]的功率可以降低大约50％。第一制冷剂压缩机[M]和[Q]的功率需求大致相等地增加。
申请人提出，具有明显低于环境温度的入口温度的氢压缩机的这种运行布置对于氢液化的现有技术来说既新颖又特别有利：
-氢压缩通常需要使用往复式压缩机，因为氢的密度对于离心式压缩机来说可能太低；考虑到往复式压缩机相对高的投资和运行成本(特别是在大型装置中需要多台压缩机并联)，由于使用低于环境温度的入口温度，往复式压缩机的功率需求将显著降低；
-氢压缩机在明显低于环境温度的入口温度下的运行增加了入口密度；例如，在-120℃时，入口密度大约是环境温度下密度的2倍，有利于在氢液化中使用离心压缩。
在图3/3(图3)所示的本发明的第三方面中，通过在闭合回路中的一个或多个级中的第二制冷剂的膨胀来提供在氢液化单元[E]中进一步冷却和液化氢流所需的部分或全部制冷。通过这种布置，在氢液化单元[E]中通过流[6]的一部分的膨胀而产生的制冷量可以大大减少或甚至消除，因此流[8]的流速和压缩机[A]所需的功率可以明显低于图1/3(图1)所示的流程图。
根据本发明的第三方面：
-在热交换器[B]、[C]和[D]中连续冷却第二制冷剂流[11]，以形成流[14]，该流通常具有与氢液化器单元[E]的氢入口流[6]相同的温度；
-除了关于本发明的主要方面描述的并且在图1/3(图1)中示出的氢液化单元[E]的典型内部布置之外，氢液化单元[E]通常还包括：将流[14]分成两部分；在第一膨胀器中冷却第一部分[e-11]以形成出口流[e-12]；在第一热交换器中冷却第二部分[e-13]以形成流[e-14]；在第一热交换器中再加热流[e-14]以形成流[e-15]；在第二膨胀器中进一步冷却流[e-12]以形成出口流[e-16]；在第二热交换器中再加热流[e-16]以形成流[e-17]；以及合并流[e-15]和[e-17]以形成流[15]；
-流[15]以低于流[14]的压力离开氢液化器单元[E]；
-然后在热交换器[D]、[C]和[B]中连续再加热流[15]，以在接近环境温度下形成再加热流[18]；
-然后在压缩机[F]中再压缩流[18]，以在冷却上述第二制冷剂[11]后形成。
第二制冷剂可包括氢、氦或氖，或其混合物。
在使用氢作为第二制冷剂的情况下，在第二制冷剂回路中没有转化催化剂的情况下，预计邻位氢不会显著转化为对位氢。由于在本发明的第三方面中得到的上述较低的流[6]的流量，在氢液化器单元[E]中流过转化催化剂的氢的流量可能低于图1/3(图1)所示的本发明的主要方面中的氢的流量，因此也可能减少邻位氢向对位氢转化催化剂的量。
本发明已经通过广泛使用的工艺模拟软件进行了广泛的模拟。
具体实施方式
将参照附图描述本发明，附图中示出了对根据本发明的工艺的实施例进行说明的流程图。
确切的流程图可能会有变化，但通常会包含这些基本元件。
在图1/3(图1)所示的本发明的第一实施例中，将压力为25巴的待液化氢的进料流[1]送入压缩机[A]。压缩机还接收以下描述的循环氢流[2]。冷却后的进料氢和循环氢的合并流[3]以75巴的压力从压缩机中排出。
通过穿过热交换器[B]的第一热通道，合并流[3]被冷却至-50℃以形成流[4]；然后通过穿过热交换器[C]的第一热通道，合并流被冷却至-120℃以形成流[5]；如下所述，通过甲烷制冷剂的闭合回路提供必要的制冷。
通过蒸发低压甲烷制冷剂流进一步将来自热交换器[C]的出口流[5]冷却至-158℃以形成流[6]。
流[6]然后流动到氢液化单元[E]，该氢液化单元包括一个或多个氢膨胀器、一个或多个热交换器以及一个或多个邻位-对位氢催化转化级。
氢液化单元[E]具有温度为-244℃、压力为7.5巴的液态氢出口流[7]，和温度为-161℃、压力为6.8巴的气态氢流的出口流[8]。
首先在热交换器[D]的冷通道中对流[8]进行再加热以形成温度为-123℃的流[9]，然后在热交换器[C]的第一冷通道中对流进行进一步再加热以形成温度为-53℃的流[10]，然后在热交换器[B]的第一冷通道中对流进行进一步再加热，在接近环境温度下被再加热的流形成上述氢循环流[2]。
上述含有甲烷制冷剂的封闭制冷回路在制冷剂压缩机[M]的排放处具有压力为90巴的流[21]。
来自压缩机[M]的出口流[21]被分成第一部分[22]和第二部分[25]。
第一部分[22]进入第一制冷剂气体膨胀器[L]，该第一制冷剂气体膨胀器具有压力为26巴、温度为-54℃的出口流[23]。第二部分[25]穿过热交换器[B]的第二热通道，该第二热通道具有出口流[26]，该出口流具有与上述氢流[4]相同的-50℃的出口温度。
在热交换器[B]的第二冷通道中将流[23]再加热至接近环境温度。在上述制冷剂气体流[21]冷却后，被再加热的流[24]在接近环境温度下作为第一组分流动到制冷剂压缩机[M]。
来自热交换器[B]的出口流[26]流动到第二制冷剂气体膨胀器[N]，该第二制冷剂气体膨胀器具有压力为10巴、温度为-124℃且含有蒸汽和液体的出口流[27]。
在蒸汽/液体分离器[O]中分离流[27]以形成蒸汽流[28]和液体流[29]。
在阀[P]中将液体流[29]减压至接近大气压力，以在出口流[30]中形成温度为-158℃的液体和蒸汽混合物。
流[30]在热交换器(D)的第二冷通道中被完全蒸发和再加热，以形成出口蒸汽流[31]，该出口蒸汽流具有与上述氢流[9]相同的-123℃的温度。流[31]被制冷剂压缩机[Q]压缩，该制冷剂压缩机的出口流[32]具有与流[28]相同的9.7巴的压力。然后将流[28]和[33]合并以形成流[34]。
首先在热交换器[C]的第二冷通道中再加热流[34]，以形成温度为-53℃的流[35]，然后在热交换器[B]的第三冷通道中再加热流。在上述制冷剂气体流[21]冷却后，被再加热的流[36]在接近环境温度下作为第二组分流动到压缩机[M]。
将参照表示本发明的第二实施例的附图2/3(图2)进一步描述本发明。在上面的概述中描述的该第二实施例包括第一实施例的变型，其中，氢再循环压缩机[A]接收具有明显低于环境吸入温度的入口流。
在该第二实施例的示例中，氢再循环流[9]以-123℃的温度和6.6巴的压力直接地流动到压缩机[A]。来自压缩机[A]的出口流[3]的温度随后被降低至接近环境温度。

Claims (13)

1.一种用于液化氢气的方法，所述工艺包括：
-提供氢进料气体流[1]；
-以1巴至50巴的压力提供再循环氢气流[2]；
-使流[1]和[2]进入氢压缩机[A]，所述压缩机具有合并排放流[3]，所述合并排放流的压力介于10巴至200巴之间；
-在热交换器[B]的第一热通道中冷却所述合并排放流[3]，所述热通道具有出口流[4]；
-在热交换器[C]的第一热通道中冷却所述流[4]，所述热通道具有出口流[5]；
-在热交换器[D]的第一热通道中冷却所述流[5]，所述热通道具有出口流[6]；
-使流[6]进入氢液化器单元[E]，所述氢液化器单元包括一个或多个氢气膨胀器、一个或多个热交换器以及将邻位氢催化转化为对位氢的一个或多个级；氢液化器具有温度介于-240℃至-255℃之间的液态氢出口流[7]和压力介于1巴至20巴之间的气态氢出口流[8]；
-在热交换器[D]的第一冷通道中再加热流[8]，所述冷通道具有出口流[9]，然后在热交换器[C]的第一冷通道中再加热所述流，所述冷通道具有出口流[10]，然后在热交换器[B]的第一冷通道中再加热所述流，来自热交换器[B]的被再加热的所述流形成上面所述的再循环氢气流[2]；
-提供压力为10巴至150巴的制冷剂气体流[21]；
-将制冷剂气体流[21]分成第一部分[22]和第二部分[25]；
-使所述第一部分[22]进入第一制冷剂气体膨胀器[L]，来自所述第一制冷剂气体膨胀器的出口流[23]具有介于5巴至50巴之间的压力；
-在热交换器[B]的第二冷通道中再加热第一制冷剂气体膨胀器出口流[23]以形成再加热流[24]；
-在压缩机[M]中将所述再加热流[24]压缩至10巴至150巴的压力，以形成上面所述的制冷剂气体[21]的第一组分；
-使所述制冷剂气体的所述第二部分[25]进入热交换器[B]的第二热通道，所述第二热通道具有出口流[26]；
-使制冷剂气体[26]的冷却的所述第二部分进入第二制冷剂气体膨胀器[N]，来自所述第二制冷剂气体膨胀器的出口流[27]具有介于3巴至50巴之间的压力，并且包括蒸汽和液体的混合物；
-在蒸汽/液体分离器[O]中分离第二气体膨胀器[N]的所述出口流[27]，以形成蒸汽流[28]和液体流[29]；
-在阀[P]中对所述液体流[29]进行减压以形成压力介于0.5巴至10巴之间的流[30]；
-在热交换器(D)的第二冷通道中对流[30]进行蒸发和再加热，以形成出口蒸汽流[31]；
-通过低压制冷剂压缩机[Q]将流[31]压缩至与流[28]的压力相同的压力，所述低压制冷剂压缩机具有出口流[32]；
-合并流[28]和流[32]以形成流[34]；
-在热交换器[C]的第二冷通道中再加热流[34]以形成流[35]，然后在热交换器[B]的第三冷通道中再加热所述流以形成流[36]；
-在压缩机[M]中将被再加热的所述流[36]压缩至10巴至150巴的压力，以形成上面所述的制冷剂气体[21]的第二组分。
2.根据权利要求1所述的方法，其中，来自压缩机[A]的合并排放流[3]具有介于20巴至100巴之间的压力。
3.根据权利要求1或2所述的方法，其中，所述流[30]的压力介于1巴至3巴之间。
4.根据权利要求1至3所述的方法，其中，所述制冷剂气体是甲烷或富含甲烷的气体。
5.根据权利要求4所述的方法，其中，来自第二气体膨胀器[N]的所述出口流[27]的压力介于10巴至50巴之间。
6.根据权利要求1至3所述的方法，其中，所述制冷剂气体是氮气。
7.根据权利要求6所述的方法，其中，来自第二气体膨胀器[N]的所述出口流[27]的压力介于3巴至30巴之间。
8.根据权利要求1至3所述的方法，其中，所述制冷剂气体是甲烷和氮气的混合物。
9.根据权利要求1至3所述的方法，其中，在第一制冷剂气体膨胀器[L]中流动的所述制冷剂气体[21]是甲烷或富含甲烷的气体，而在第二制冷剂气体膨胀器[N]、分离器[O]和阀[P]中流动的所述制冷剂气体[26]是氮气。
10.根据前述权利要求中任一项所述的方法，其中，压缩机[A]的入口流[2]的温度介于-200℃至40℃之间。
11.根据权利要求10所述的方法，其中，压缩机[A]的所述入口流直接取自所述氢液化器单元[E]的出口流[8]，或来自所述热交换器[D]或[C]的第一冷通道的出口。
12.根据前述权利要求中任一项所述的方法，其中，提供接近环境温度的第二制冷剂气体流[11]；在热交换器[B]的第三热通道中冷却所述流[11]以形成出口流[12]；在热交换器[C]的第二热通道中冷却所述流[12]以形成出口流[13]；在热交换器[D]的第二热通道中冷却所述流[13]以形成出口流[14]；使所述流[14]进入氢液化单元[E]，在所述氢液化单元中，在作为流[15]离开[E]之前，流[14]穿过一个或多个膨胀级以提供制冷；在热交换器[D]的第三冷通道中再加热流[15]以形成流[16]；在热交换器[C]的第三冷通道中进一步再加热流[16]以形成流[17]；以及在热交换器[B]的第四冷通道中进一步再加热流[17]以形成流[18]；以及在压缩机[F]中再压缩流[18]以形成所述流[11]。
13.根据权利要求12所述的方法，其中，所述第二制冷剂气体是氢、氦，或者氢或氦与氖的混合物。
CN202180074434.4A 2020-11-21 2021-10-13 生产液化氢的方法 Pending CN116507870A (zh)

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