CN108441261B - 一种基于氩循环制冷含氮富甲烷气分离***及分离方法 - Google Patents

一种基于氩循环制冷含氮富甲烷气分离***及分离方法 Download PDF

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CN108441261B
CN108441261B CN201810437481.0A CN201810437481A CN108441261B CN 108441261 B CN108441261 B CN 108441261B CN 201810437481 A CN201810437481 A CN 201810437481A CN 108441261 B CN108441261 B CN 108441261B
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舒伟
张敏卿
毛文军
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Abstract

本发明涉及一种基于氩循环制冷含氮富甲烷气分离***及分离方法，分离***包括甲烷分离***和氩循环制冷***，含氮富甲烷气进入甲烷分离***后，分离的液态甲烷进入氩循环制冷***中的液态甲烷‑氩气换热器中，将液态甲烷的冷能传递给循环氩，循环氩用于为甲烷分离***中的塔顶分凝器提供冷能，实现冷能回收过程。分离方法是将液态甲烷的冷能传递给循环氩，循环氩反过来为含氮富甲烷气分离液态甲烷提供冷能。本发明的分离***以循环氩为工质，通过热泵、冷能换热器回收分离***甲烷及氮气冷能，通过部分氩气膨胀制冷补充冷能后，再利用氩气焦耳‑汤姆逊效应提高冷能品位后将其传递给含氮富甲烷气分离***，以较低制冷能耗实现高效分离。

Description

一种基于氩循环制冷含氮富甲烷气分离***及分离方法
技术领域
本发明属于含氮富甲烷工业尾气中产品回收领域技术领域，涉及一种基于氩循环制冷含氮富甲烷气分离***及分离方法。
背景技术
炼厂干气主要来源于石油加工的重油催化裂化、延迟焦化、加氢裂化、催化重整等过程，其主要成份包括氢气、氮气、甲烷、乙烯、乙烷、丙烷等，其中氢气、乙烯、乙烷等价值较高。乙烯本身即是高价值产品，氢气可回用于加氢裂化或作为产品出售，乙烷和丙烷等轻烃作为优质裂解原料可回用于乙烯装置。然而除极少数有配套乙烯装置的炼化企业采用了乙烯原料回收工艺，多数炼厂将干气作为燃料气使用。甲醇合成驰放气中主要成份包括氢气、氮气、甲烷等，部分厂家通过昂贵的甲烷化工艺，将驰放气转化为LNG，仍有相当部分将驰放气燃料气使用。将干气及驰放气直接作为燃料使用，存在高价产品的低值化使用，造成资源浪费。
干气中高价产物的分离回收通常采用吸附、吸收、膜及深冷分离中的一种或其组合。吸附法利用选择性吸附剂通过压力及温度改变实现吸附与解吸的循环，得到相对纯的某一组份。如专利CN201410220850.2，采用浅冷吸附吸收回收干气中的氢气及乙烯。吸附法收率及纯度相对偏低，装置投资及占地较大。吸收法则采用溶剂吸收进行选择性吸收，再通过精馏分离才能获得高纯产品。如专利CN201410220882.2、CN201410359774.3分别采用丁烷、戊烷、芳烃或乙腈等溶剂进行选择性吸收，回收干气中的氢气、乙烯。因溶剂特性，吸收性存在选择性不高，分离收率低的缺点，并且仍需要提供冷能进行精密分离，从而限制了该方法的应用。膜分离是利用干气中不同组份在特种膜中的渗透性差异实现组份的分离，其适于带压低氢干气中氢气的回收，但纯度不高。深冷分离一般以甲烷、乙烯丙烯丙烷为制冷剂，通过压缩、冷凝节流膨胀过程获得所需的低温冷能。深冷分离能保证产品纯度及高收率，用于干气分离可以得到聚合级的乙烯，用于驰放气分离可提高甲烷回收率，但常规深冷法操作压力高能耗大，昂贵的制冷成本制约了该方法的广泛应用，仅适于大规模处理。
天然气是优质环保燃料，通常采用液态（LNG）方式运输，在其燃烧前需要将低温深冷（常压-162℃）的液态复热变成气态，将LNG的气化冷能用于干气分离则能大大降低干气分离的成本。甲烷常压气化温度只有-162℃，此温度下甲烷很难与干气或油田伴生气中的氮气进行高清分离，致使甲烷回收率低，同时轻组分氢氮中夹带甲烷，影响氢气回收。
发明内容
本发明所要解决的技术问题是针对现有技术的不足，提供一种基于氩循环制冷含氮富甲烷气分离***及分离方法。本发明的氩循环制冷***以氩为循环工质，通过热泵、冷能换热器回收分离***甲烷及氮气冷能，通过部分氩气膨胀制冷补充冷能，再利用氩气焦耳-汤姆逊效应提高冷能品位后将其传递给含氮富甲烷气分离***，以较低制冷能耗实现高效分离，实现干气、驰放气、陆地及海洋油田伴生气、煤层气和页岩气等工业资源的高价利用，从以上气体中的甲烷回收率可达99%以上。
为解决上述问题，本发明采用如下技术方案：
一种基于氩循环制冷含氮富甲烷气分离***，包括甲烷分离***和氩循环制冷***，含氮富甲烷气进入所述甲烷分离***后，分离的液态甲烷自甲烷精馏塔的塔底流出后进入所述氩循环制冷***中的液态甲烷-氩气换热器中，将液态甲烷的冷能传递给循环氩，循环氩用于为甲烷分离***中的塔顶分凝器提供冷能，实现含氮富甲烷气的分离用冷能回收过程。
进一步地，所述甲烷分离***包括甲烷精馏塔、塔底再沸器和塔顶分凝器；再沸器的一端连接有输送含氮富甲烷气的原料气管道，另一端通过甲烷精馏塔进料管道将含氮富甲烷气输送至甲烷精馏塔内。含氮富甲烷气原料作为再沸器热源，原料在再沸器内将热能传递给塔底循环液，部分塔底液气化形成气相进行分离；塔内上升气相中部分氮气在塔顶分凝器内吸收氩气冷能冷凝为液氮，形成塔内回流液实现甲烷氮气的高效分离。经过甲烷分离塔，在塔顶得到不含甲烷的轻组份，包括氮气和更轻的氢气及一氧化碳组份，塔底得到液体甲烷。
进一步地，所述氩循环制冷***包括甲烷节流膨胀阀、液态甲烷-氩气换热器、液氩节流膨胀阀、冷能换热器、循环氩气压缩机和第一水冷换热器，所述液态甲烷自甲烷节流膨胀阀流入液态甲烷-氩气换热器的吸热管路将冷能释放给的循环氩，循环氩通过液氩节流膨胀阀进入塔顶分凝器释放冷能后，通过低压冷氩气管道进入冷能换热器中再次释放冷能，然后自低压复热氩气管道进入循环氩气压缩机中压缩后，进一步提高压力，然后进入第一水冷换热器中降温预冷，通过高压氩气管道再次进入冷能换热器中降温预冷，然后进入液态甲烷-氩气换热器中再次获得冷能，实现氩循环制冷主回路。
进一步地，所述甲烷分离***中分离的气体自甲烷精馏塔的塔顶流出后进入所述冷能换热器中释放冷能，然后自复热塔顶气管道流入塔顶气利用***中。塔顶气相通过冷能换热器将冷能释放给制冷***，可以进一步回收冷能，提高冷能的利用率。复热后塔顶气相则通过管道排出***，通过变压吸附或膜分离可实现氢气一氧化碳与氮气（相对于驰放气）、氢气与氮气（相对于干气）或氢气与氦气（相对于油田伴生气）的分离，作为甲醇合成原料或加氢原料，提高驰放气和干气的利用率。甲烷气压缩冷却及塔顶气的变压吸附或膜分离可采用工业上常用技术方法进行。
进一步地，所述液态甲烷-氩气换热器的吸热管路中流出的冷甲烷气，通过冷甲烷气管道进入冷能换热器中再次释放冷能，然后自复热甲烷气管道流入甲烷利用***中。复热后的甲烷气通过管道排出***，根据用户压力要求，进行压缩和冷却后输入用户管网。
进一步地，所述氩循环制冷***中还包括氩循环制冷副回路，所述氩循环制冷副回路中包括氩气膨胀机，具体为：从氩循环制冷主回路中分出的一路循环氩气进入冷能换热器降温预冷后直接通过膨胀机膨胀端进口管道进入膨胀机内膨胀降温，再经膨胀机膨胀端出口管道回到冷能换热器释放冷能并复热后，通过膨胀机压缩端进口管道进入膨胀机压缩端提高压力并经膨胀机压缩端出口管道进入第二水冷换热器降温，然后再经过循环氩气压缩机进一步提高压力后进入第一水冷换热器降温，通过高压氩气管道进入冷能换热器降温预冷，形成氩循环制冷副回路。该***以氩为循环工质，通过热泵及冷能换热器回收甲烷及氮气冷能，通过部分氩气膨胀机制冷对氩循环制冷主回路进行冷能补充，再利用氩气焦耳-汤姆逊效应提高冷能品位后将其传递给甲烷分离***。
进一步地，所述含氮富甲烷气的来源为甲醇合成驰放气或炼油装置干气脱除乙烯后的含氮甲烷气体或陆上及海上油田伴生气脱除轻烃后的甲烷气或经过脱碳净化后的煤层气页岩气。除氮气和甲烷外，对于驰放气还包括氢气及一氧化碳；对于干气则还含氢气，在用变压吸附或膜分离方法去除氮气后均可作为原料回到原***；对于陆上及海上油田伴生气为资源的氮富甲烷原料气，除氮气和甲烷外，还含有氢气氦气，用变压吸附或膜分离方法去除氮气后，回收氢气及氦气。
进一步地，本发明还提供了基于氩循环制冷含氮富甲烷气分离***的分离方法，将含氮富甲烷气在甲烷分离***分离后，分离的液态甲烷进入所述液态甲烷-氩气换热器中，将液态甲烷的冷能传递给循环氩，循环氩用于为甲烷分离***中的塔顶分凝器提供冷能，实现含氮富甲烷气的分离。
有益效果
本发明的基于氩循环制冷含氮富甲烷分离***，以氩气为工质通过热泵、冷能换热器回收分离***甲烷及氮气冷能，通过部分氩气膨胀制冷补充冷能，再利用氩气焦耳-汤姆逊效应提高冷能品位后将其传递给分离***，以较低制冷能耗实现氮气与甲烷分离，其中甲烷精馏塔塔顶气相含有氢气一氧化碳与氮气（相对于驰放气）、氢气与氮气（相对于干气）或氢气与氦气（相对于陆上或海上油田伴生气）的分离,排出分离***后可通过变压吸附或膜分离等工业上常用技术方法脱除氮气，回收氢气氦气等高价值资源。
附图说明
图1为本发明的一种基于氩循环制冷含氮富甲烷气分离***的示意图；
其中，1-塔底再沸器、1-1-原料气管道、2-甲烷精馏塔、2-1-甲烷精馏塔进料管道、2-2-塔顶气相出料管道、2-3-塔底液相出料管道、3-塔顶分凝器、3-1-低压冷氩气管道、4-冷能换热器、4-1-复热塔顶气管道、4-2-复热甲烷气管道、4-3-低压复热氩气管道、5-循环氩气压缩机、6-第一水冷换热器、6-1-高压预冷氩气管道、7-液态甲烷-氩气换热器、7-1-高压冷氩气管道、7-2-冷甲烷气管道、8-液氩节流膨胀阀、8-1-高压液氩管道、8-2-低压液氩管道、9-氩气膨胀机、9-1-膨胀机膨胀端进口管道、9-2-膨胀机膨胀端出口管道、9-3-膨胀机压缩端进口管道、9-4-膨胀机压缩端出口管道、10-第二水冷换热器、11-甲烷节流膨胀阀。
具体实施方式
下面结合具体实施方式，进一步阐述本发明。应理解，这些实施例仅用于说明本发明而不用于限制本发明的范围。此外应理解，在阅读了本发明讲授的内容之后，本领域技术人员可以对本发明作各种改动或修改，这些等价形式同样落于本申请所附权利要求书所限定的范围。
实施例1
一种基于氩循环制冷含氮富甲烷气分离***，包括甲烷分离***和氩循环制冷***，含氮富甲烷气进入甲烷分离***后，分离的液态甲烷自甲烷精馏塔的塔底流出后进入氩循环制冷***中的液态甲烷-氩气换热器7中，将液态甲烷的冷能传递给循环氩，循环氩用于为甲烷分离***中的塔顶分凝器3提供冷能，实现含氮富甲烷气的分离用冷能回收过程。
甲烷分离***包括甲烷精馏塔2、再沸器1和塔顶分凝器3；再沸器1的一端连接有输送含氮富甲烷气的原料气管道1-1，另一端通过甲烷精馏塔进料管道2-1将含氮富甲烷气输送至甲烷精馏塔2内。含氮富甲烷气原料作为再沸器1热源，原料在再沸器1内将热能传递给塔底循环液，部分塔底液气化形成气相进行分离；塔内上升气相中部分氮气在塔顶分凝器3内吸收氩气冷能冷凝为液氮，形成塔内回流液实现甲烷氮气的高效分离。经过甲烷精馏塔3，在塔顶通过塔顶气相出料管道2-2得到不含甲烷的轻组份，包括氮气和更轻的氢气及一氧化碳等组份，塔底通过塔底液相出料管道2-3得到液体甲烷。
进一步地，氩循环制冷***包括甲烷节流膨胀阀11、液态甲烷-氩气换热器7、液氩节流膨胀阀8、冷能换热器4、循环氩气压缩机5和第一水冷换热器6。液态甲烷自甲烷节流膨胀阀11流入液态甲烷-氩气换热器7的吸热管路将冷能释放给的循环氩，循环氩在通过液氩节流膨胀阀8之前的管道为高压液氩管道8-1，通过液氩节流膨胀阀8之后的管道为低压液氩管道8-2；循环氩通过液氩节流膨胀阀8进入塔顶分凝器3释放冷能后，通过低压冷氩气管道3-1进入冷能换热器4中再次释放冷能，然后自低压复热氩气管道4-3进入循环氩气压缩机5中压缩后，进入第一水冷换热器6中降温预冷，通过高压氩气管道再次进入冷能换热器4中降温预冷，然后通过高压冷氩气管道7-1进入液态甲烷-氩气换热器7中再次获得冷能，实现氩循环制冷主回路。
进一步地，甲烷分离***中分离的气体自甲烷精馏塔2的塔顶流出后进入冷能换热器4中释放冷能，然后自复热塔顶气管道4-1流入塔顶气利用***中。塔顶气相通过冷能换热器4将冷能释放给制冷***，可以进一步回收冷能，提高冷能的利用率。复热后塔顶气相则通过管道排出***，通过变压吸附或膜分离可实现氮气与其它高值气体氢气一氧化碳（相对于驰放气）、氢气（相对于干气）或氢气与氦气（相对于油田伴生气）的分离，提高原料气的利用率。甲烷气压缩冷却及塔顶气的变压吸附或膜分离可采用工业上常用技术方法进行。
进一步地，液态甲烷-氩气换热器7的吸热管路中流出的冷甲烷气，通过冷甲烷气管道7-2进入冷能换热器4中再次释放冷能，然后自复热甲烷气管道4-2流入甲烷利用***中。复热后的甲烷气通过管道排出***，根据用户压力要求，进行压缩和冷却后输入用户管网。
进一步地，氩循环制冷***中还包括氩循环制冷副回路，氩循环制冷副回路中包括氩气膨胀机9，具体为：从氩循环制冷主回路中分出的一路循环氩气进入冷能换热器4降温预冷后直接通过膨胀机膨胀端进口管道9-1进入膨胀机9内膨胀降温，再经膨胀机膨胀端出口管道9-2回到冷能换热器4释放冷能并复热后，通过膨胀机压缩端进口管道9-3进入膨胀机压缩端提高压力并经膨胀机压缩端出口管道9-4进入第二水冷换热器10降温，然后再经过循环氩气压缩机5进一步提高压力后进入第一水冷换热器6降温，通过高压预冷氩气管道6-1进入冷能换热器4降温预冷，形成氩循环制冷副回路。该***以氩为循环工质，通过热泵及冷能换热器4回收甲烷及氮气冷能，部分氩气通过膨胀机9制冷对氩循环制冷主回路进行冷能补充，再利用氩气焦耳-汤姆逊效应提高冷能品位后将其传递给甲烷分离***。
进一步地，含氮富甲烷气的来源为甲醇合成驰放气或炼油装置干气脱除乙烯后的含氮甲烷气体或陆上及海上油田伴生气脱除轻烃后的甲烷气或经过脱碳净化后的煤层气页岩气。除氮气和甲烷外，对于驰放气还包括氢气及一氧化碳；对于干气则还含氢气，在用变压吸附或膜分离方法去除氮气后均可作为原料回到原***；对于陆上及海上油田伴生气为资源的氮富甲烷原料气，除氮气和甲烷外，还含有氢气氦气，用变压吸附或膜分离方法去除氮气后，回收氢气及氦气。
进一步地，本发明还提供了基于氩循环制冷含氮富甲烷气分离***的分离方法，将含氮富甲烷气在甲烷分离***分离后，分离的液态甲烷进入液态甲烷-氩气换热器7中，将液态甲烷的冷能传递给循环氩，循环氩用于为甲烷分离***中的塔顶分凝器3提供冷能，实现含氮富甲烷气的分离。
本发明的氩循环制冷***以氩为循环工质，通过热泵、冷能换热器回收分离***甲烷及氮气冷能，通过部分氩气膨胀制冷补充冷能，再利用氩气焦耳-汤姆逊效应提高冷能品位后将其传递给含氮富甲烷气分离***，以较低制冷能耗实现高效分离，实现干气、驰放气等工业尾气资源的高价利用，从陆地及海洋油田伴生气中回收氢气氦气甲烷及轻烃，甲烷回收率可达99%以上。
本发明的氩循环制冷***采用液态甲烷-氩气换热器，以氩气为工质通过热泵回收LNG冷能，利用氩气焦耳-汤姆逊效应提高冷能品位后传递给被冷却介质，可以有效提高LNG冷能利用率，使LNG冷能利用率提高到９０％以上，更好的实现绿色环保理念，该节能效果清楚记载在本申请人在申请号2018100218512或申请号2018200373138的专利文本中。
本发明公开和提出的方法，本领域技术人员可通过借鉴本文内容，适当改变条件路线等环节实现，尽管本发明的方法和制备技术已通过较佳实施例子进行了描述，相关技术人员明显能在不脱离本发明内容、精神和范围内对本文的方法和技术路线进行改动或重新组合，来实现最终的制备技术。特别需要指出的是，所有相类似的替换和改动对本领域技术人员来说是显而易见的，他们都被视为包括在本发明精神、范围和内容中。

Claims (3)

1.一种基于氩循环制冷含氮富甲烷气分离***，其特征是：包括甲烷分离***和氩循环制冷***，含氮富甲烷气进入所述甲烷分离***后，分离的液态甲烷自甲烷精馏塔的塔底流出后进入所述氩循环制冷***中的液态甲烷-氩气换热器中，将液态甲烷的冷能传递给循环氩，循环氩用于为甲烷分离***中的塔顶分凝器提供冷能，实现含氮富甲烷气的分离用冷能回收过程；
所述甲烷分离***包括甲烷精馏塔、塔底再沸器和塔顶分凝器；再沸器的一端连接有输送含氮富甲烷气的原料气管道，另一端通过甲烷精馏塔进料管道将含氮富甲烷气输送至甲烷精馏塔内；
采用氩做为制冷循环工质，所述氩循环制冷***包括甲烷节流膨胀阀、液态甲烷-氩气换热器、液氩节流膨胀阀、冷能换热器、循环氩气压缩机和第一水冷换热器，所述液态甲烷自甲烷节流膨胀阀流入液态甲烷-氩气换热器的吸热管路将冷能释放给循环氩，循环氩通过液氩节流膨胀阀进入塔顶分凝器释放冷能后，通过低压冷氩气管道进入冷能换热器中再次释放冷能，然后自低压复热氩气管道进入循环氩气压缩机中压缩后，进一步提高压力，然后进入第一水冷换热器中降温预冷，通过高压预冷氩气管道再次进入冷能换热器中降温预冷，然后进入液态甲烷-氩气换热器中再次获得冷能，实现氩循环制冷主回路；
所述甲烷分离***中分离的气体自甲烷精馏塔的塔顶流出后进入所述冷能换热器中释放冷能，然后自复热塔顶气管道流入塔顶气利用或排放***中；
所述液态甲烷-氩气换热器的吸热管路中流出的冷甲烷气，通过冷甲烷气管道进入冷能换热器中再次释放冷能，然后自复热甲烷气管道流入甲烷利用***中；
所述氩循环制冷***中还包括氩循环制冷副回路，所述氩循环制冷副回路中包括氩气膨胀机，具体为：从氩循环制冷主回路中分出的一路循环氩气进入冷能换热器降温预冷后直接通过膨胀机膨胀端进口管道进入膨胀机内膨胀降温，再经膨胀机膨胀端出口管道回到冷能换热器释放冷能并复热后，通过膨胀机压缩端进口管道进入膨胀机压缩端提高压力并经膨胀机压缩端出口管道进入第二水冷换热器降温，然后再经过循环氩气压缩机进一步提高压力后进入第一水冷换热器降温，通过高压预冷氩气管道进入冷能换热器降温预冷，形成氩循环制冷副回路。
2.根据权利要求1所述的一种基于氩循环制冷含氮富甲烷气分离***，其特征是：所述含氮富甲烷气的来源为甲醇合成驰放气或炼油装置干气脱除乙烯后的含氮甲烷气体或陆上及海上油田伴生气脱除轻烃后的甲烷气或经过脱碳净化后的煤层气页岩气。
3.根据权利要求1-2任一所述的基于氩循环制冷含氮富甲烷气分离***的分离方法，其特征是：将含氮富甲烷气在甲烷分离***分离后，分离的液态甲烷进入所述液态甲烷-氩气换热器中，将液态甲烷的冷能传递给循环氩，循环氩用于为甲烷分离***中的塔顶分凝器提供冷能，实现含氮富甲烷气的分离。
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