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TWI840733B - 利用與變壓吸附單元及/或低溫分離系統整合的氣體分離膜之增強氫氣回收技術 - Google Patents

利用與變壓吸附單元及/或低溫分離系統整合的氣體分離膜之增強氫氣回收技術 Download PDF

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TWI840733B
TWI840733B TW111100805A TW111100805A TWI840733B TW I840733 B TWI840733 B TW I840733B TW 111100805 A TW111100805 A TW 111100805A TW 111100805 A TW111100805 A TW 111100805A TW I840733 B TWI840733 B TW I840733B
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swing adsorption
tail gas
pressure swing
hydrogen
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TW202315673A (zh
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謝哈爾 特瓦里
羅納德 Ｍ 維那
桑尼爾 潘迪托
迪尼斯 馬隆尼
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美商魯瑪斯科技有限責任公司
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Abstract

回收氫氣之方法及系統可包括將包含氫氣及額外氣體之氣流饋入至變壓吸附(PSA)系統及將包含氫氣之膜滲透物流饋入至該PSA系統。在該PSA系統中，一部分該氫氣可與該等額外氣體分離以回收氫氣產物流及包含未分離氫氣及該等額外氣體之PSA尾氣流。該PSA尾氣流可饋入至膜分離單元以用於將氫氣與該等額外氣體分離且回收(i)饋入至該PSA系統之該包含氫氣之膜滲透物流及(ii)包含該等額外氣體之膜尾氣流。本文實施例可另外包括致冷系統，用於部分地冷凝饋料氣體流及該PSA尾氣流中之一或二者，從而增強該膜分離單元之效率。

Description

利用與變壓吸附單元及/或低溫分離系統整合的氣體分離膜之增強氫氣回收技術
發明領域
本揭露內容之實施例大體上係關於自氣流中回收氫氣。
發明背景
許多石油化工過程使用或產生氫氣(H2)，且通常回收未反應或所產生之氫氣以用於在石油化工廠內再循環或使用。當前，通常使用變壓吸附(PSA)單元或低溫分離單元自混合氣流中回收氫氣，同時將所得尾氣投送至燃料氣體池。
PSA及低溫分離對可回收之H2的最大量具有技術限制。始終存在一些氫氣在尾氣流中損失。此等組態之一個主要缺點為氫氣流失至低價值的料流中，導致該等單元之整體操作費用增加。
發明概要
本文實施例將氣體分離膜與PSA及/或低溫分離整合以增強氫氣之整體回收率，且將高價值氫氣至低價值燃料氣體流的損失最小化。此類額外氫氣回收可為操作費用節省提供顯著益處。此亦將二氧化碳(CO2)濃縮於所得尾氣 中，其使尾氣流中之碳捕獲更加高效且經濟。
在一個態樣中，本文所揭露之實施例係關於用於回收氫氣之方法。用於回收氫氣之方法可包括將包含氫氣及額外氣體之氣流饋入至變壓吸附(PSA)系統及將包含氫氣之膜滲透物流饋入至該PSA系統。在該PSA系統中，一部分氫氣可與額外氣體分離以回收氫氣產物流及包含未分離氫氣及額外氣體之PSA尾氣流。該PSA尾氣流可饋入至膜分離單元以用於將氫氣與額外氣體分離且回收(i)饋入至該PSA系統之該包含氫氣之膜滲透物流及(ii)包含該等額外氣體之膜尾氣流。
在一些實施例中，方法可進一步包括在膜分離單元之上游壓縮變壓吸附尾氣流。在一些實施例中，方法可進一步包括在變壓吸附系統之上游壓縮膜滲透物流。本文方法之實施例可另外包括部分地冷凝饋料氣體流及PSA尾氣流中之一或二者。
在另一態樣中，本文所揭露之實施例係關於用於回收氫氣之系統。該系統可包括用於將包含氫氣及額外氣體之氣流饋入至變壓吸附系統的流動管線，以及用於將包含氫氣之膜滲透物流饋入至變壓吸附系統的流動管線。該系統亦包括變壓吸附系統，其可經組態以用於將一部分氫氣與額外氣體分離且回收氫氣產物流及包含未分離氫氣及額外氣體之變壓吸附尾氣流。可提供流動管線以用於將變壓吸附尾氣流饋入至膜分離單元，該膜分離單元可經組態以用於將氫氣與額外氣體分離以回收(i)饋入至變壓吸附系統之包含氫氣的膜滲透物流及(ii)包含額外氣體之膜尾氣流。
在一些實施例中，系統亦可包括用於在膜分離單元之上游壓縮變壓吸附尾氣流的壓縮機。在一些實施例中，系統可進一步包括用於在變壓吸附系統之上游壓縮膜滲透物流的壓縮機。本文系統之實施例可另外包括用於部分地冷凝饋料氣體流及PSA尾氣流中之一或二者的致冷/分離系統。
其他態樣及優點將自以下描述及所附申請專利範圍而顯而易見。
1:製程氣體或廢氣流，饋料流，流動料流
2:製程氣體或廢氣流，流動料流
3:氫氣產物，氫氣產物流
4:剩餘氣體，料流，流動料流，剩餘氣流，PSA尾氣，PSA尾氣流
5:剩餘氣體，料流，流動料流，剩餘氣流
6:尾氣流，滯留物
7:流動料流，氫氣滲透物，滲透物流，富含氫氣之滲透物流，富含氫氣之滲透物，尾氣流
8:滲透物流
10:製程氣體或廢氣流
12,22:PSA單元
14:氫氣產物
16:尾氣流
24:膜分離系統，膜分離單元
26,28:壓縮機
31:低溫分離系統
32:饋料流，氣流，製程氣體流
33,45:冷卻器，交換器
35:饋料流
37,43:分離器，氣液分離器
39:底部液體流，流動管線
41:頂部流，蒸氣
47:料流
49:頂部流，第二頂部流
50:第二底部流，流動管線
51:PSA尾氣流，剩餘氣流
55:流動料流，流動管線，饋料
57:冷凝流
59:燃料氣體產物流
圖1為典型變壓吸附系統之簡化方法流程圖。
圖2及圖3為根據本文所揭露之一或多個實施例的用於回收氫氣之整合系統的簡化方法流程圖。
較佳實施例之詳細說明
本文實施例尤其針對自混合氣流(諸如來自石油化工過程之製程氣體、廢氣、排氣或尾氣流)之氫氣回收。饋入以用於氫氣回收之混合氣體可包括例如氫氣、二氧化碳、一氧化碳、硫化氫、硫氧化物、氮氣、氧氣、甲烷、乙烷、乙烯及/或丙烷以及其他組分。儘管注意到石油化工料流，但本文所描述之實施例可適用於任何含氫氣流，期望自該含氫氣流中回收氫氣。
目前先進技術利用獨立PSA單元以自過程或廢氣流中回收H2。本文實施例整合PSA與膜系統，或整合PSA及低溫分離系統與膜系統以改進整體H2回收。因此，就氫氣回收參數及回收區塊之組態而言，本文實施例不同於目前先進技術。
本文實施例可利用膜及PSA將本文中所描述之系統定位在氣流上以回收通常在尾氣流中損失之H2。可將來自膜之滲透物再循環返回至PSA以額外回收H2。在一些實施例中，低溫分離可用於改善膜系統的饋料品質。
典型先前技術PSA系統之簡單程序方塊圖展示於圖1中。製程氣體或廢氣流10(其可為任何用於H2回收之氣流)可在適當壓力下饋入至PSA單元12，以用於回收氫氣產物14。包括任何未經回收之H2的剩餘氣體係作為尾氣流16投送，該尾氣流通常用作單元中之燃料氣體。如上文所提及，自PSA單元中整體回收氫氣會導致尾氣流16中氫氣之大量損失。PSA單元通常可回收饋料 流中85-90%之氫氣，而其餘的氫氣則在尾氣中永久地損失。
本文實施例可藉由在回收系統內恰當地併入膜分離來增強尾氣流中H2之回收。尾氣可在適當壓力下饋入至膜分離單元。必要時，可利用壓縮機對膜系統所需之氣體進行加壓，以實現目標H2回收及純度。來自膜之富含氫氣的滲透物流可隨後再循環返回至PSA單元以便額外回收最終PSA產物中之H2，同時滯留物流可作為尾氣流自複合體回收且可用作燃料氣體流，經投送以用於碳捕獲或用於一些其他目的。
現參看圖2，繪示根據本文實施例之用於回收氫氣之系統的簡化方法流程圖。製程氣體或廢氣流1、2(其可為任何用於H2回收之氣流)可在適當壓力(諸如25至35巴表壓(barg))下饋入至PSA單元22，以回收氫氣產物3及剩餘氣體4。
包括任何未經回收之H2之料流4中的剩餘氣體可經由流動料流4投送至膜分離系統24。必要時，壓縮機26可用於增加料流4中剩餘氣體之壓力，從而產生可饋入至膜分離系統24之經加壓之剩餘氣流5。舉例而言，剩餘氣體可在1至5巴表壓範圍內之壓力下在料流4中回收，且剩餘氣體之壓力可增加至10至20巴表壓範圍內之壓力，且隨後經由流動料流5饋入至膜分離系統24。
在膜分離系統24中，膜用於將氫氣與剩餘氣流4、5中之其他氣體分離。氫氣滲透物可經由流動料流7回收，而滯留物流(不滲透通過膜之氣體)可作為尾氣流6回收。氫氣滲透物7可隨後再循環至變壓吸附單元22以用於與饋料流1一起回收氫氣。必要時，壓縮機28可用於增加滲透物流7中之氫氣壓力，從而產生可饋入至PSA單元22的經加壓之滲透物流8。舉例而言，富含氫氣之滲透物流7可在1至2巴表壓範圍內之壓力下自膜分離系統24回收且可再循環返回至PSA單元以便額外回收最終產物中之氫氣。滯留物流，亦即尾氣流 6可在較高壓力下回收，諸如在8至18巴表壓範圍內，且來自複合體之此尾氣流可用作燃料氣體流，經投送以用於碳捕獲，或用作一些其他目的氣體。
儘管可使用主要回收滲透物中之H2的膜，但一些其他氣體亦可與滲透物流7中之H2一起回收。此等氣體將在系統中形成一個穩態濃度，且最終在PSA單元中移除且最終經由尾氣流6離開系統。
膜分離系統24可回收PSA尾氣4中之70%至90%的氫氣，從而使得類似於圖2中所描繪之系統的整體氫氣回收率在96%至99%範圍內。
在一些實施例中，製程氣體或廢氣可包括可冷凝組分，諸如輕烴(甲烷、乙烷等)或其他較重氣體。在一些此類實施例中，可在來自PSA單元之尾氣流上利用低溫分離以冷凝較重的烴，而輕餾分可在膜系統中處理。在膜單元中處理較高純度H2氣流可提供較佳的H2回收及純度。較高純度H2之益處亦可用於在較低壓力下操作膜系統，同時達成類似於在無冷卻器之組態中達成的氫氣回收。低溫分離亦可有利地降低可影響膜之效能或與膜材料不相容之組分的濃度。
現參看圖3，說明根據本文實施例之整合低溫分離、PSA及膜分離以用於回收氫氣之系統的簡化方法流程圖，其中相同編號表示相同部件。
類似於圖2之實施例，製程氣體或廢氣流1、2(其可為任何用於H2回收之氣流)可在適當壓力下饋入至PSA單元22，以回收氫氣產物3。包括任何未經回收之H2之剩餘氣體可經由流動料流4投送至膜分離系統24。在膜分離系統24中，膜用以將氫氣與剩餘氣流4中之其他氣體分離。氫氣滲透物可經由流動料流7回收，而滯留物流(不滲透通過膜之氣體)可作為尾氣流6回收。氫氣滲透物7可隨後與製程氣體或廢氣流1組合且再循環至變壓吸附單元22以經由流動管線2回收氫氣。
為了增強PSA單元22及膜分離系統24中之每一者中的分離，可 使用低溫分離系統31。饋料流32(諸如包括氫氣及可冷凝組分(諸如輕烴)之貧乏的製程氣體或廢氣流)可在冷卻器33中冷卻，從而降低氣流32之溫度且冷凝可冷凝組分之一部分。所得經冷卻之饋料流35可饋入至氣液分離器37，諸如驟沸桶、蒸餾塔或其類似物，以自蒸氣中分離任何冷凝組分。冷凝組分可作為底部液體流39回收，且未冷凝之蒸氣可作為頂部流41回收。頂部流41接著可通過冷卻器33，從而產生饋入至PSA單元22之過程氣流或廢氣流1。
除未經回收之氫氣以外，PSA尾氣流4亦可含有可冷凝組分，諸如在氣液分離器37中未冷凝且回收之任何輕烴。PSA尾氣流4可經冷卻以冷凝至少一部分可冷凝組分且饋入至第二氣液分離器43，回收第二頂部流49及第二底部流50。
PSA尾氣流之冷卻可例如使用冷卻器33及/或第二冷卻器45中之交叉交換進行。在一些實施例中，PSA尾氣流經冷卻器33初始處理，接著經由料流47饋入至冷卻器45且與第二氣液分離器43頂部流49交叉交換。在交叉交換之後，經冷卻之PSA尾氣流51可饋入至第二氣液分離器43以用於自未經冷凝之PSA尾氣組分(經由頂部流49回收)分離冷凝組分(經由流動管線50回收)。
在冷卻器45及/或冷卻器33中之交叉交換之後，頂部流49(未經冷凝之PSA尾氣)可經由流動料流55饋入至膜分離單元24且如上文所描述進行處理。經由流動管線39、50自分離器37、43回收之冷凝組分可經組合，形成組合之冷凝流57。組合之冷凝流57可膨脹或以其他方式用於冷卻器33中之交叉交換，且回收作為燃料氣體產物流59。
雖然未在圖3中說明，但冷卻器33、45中之一或二者可包括致冷劑饋料流，以提供所需料流之所需致冷及冷卻。另外或替代地，可壓縮及/或膨脹各種料流以在冷卻器33、45內提供所要量之致冷，以產生部分冷凝。
舉例而言，使用適當的致冷劑(諸如丙烯及/或乙烯)或由致冷劑流 或過程流提供之任何致冷組合，在壓力為20至30巴表壓的貧乏製程氣體流32在冷卻器33中冷卻至-37℃至-60℃之溫度。接著經冷卻之饋料流35可在20至30巴表壓壓力下操作之氣液分離器37中驟沸。將來自分離器之蒸氣41加熱回35℃至45℃範圍內之溫度，之後經由流動料流1、2將其遞送至PSA單元22以用於回收氫氣產物流3。
來自PSA單元22之剩餘氣體4在一系列冷卻器中使用甲烷/丙烯/乙烯或任何致冷組合進一步冷卻至-60℃至-98℃範圍內之溫度。舉例而言，剩餘氣體4可首先在交換器33中冷卻且在交換器45中進一步冷卻，從而產生經冷卻之剩餘氣流51。剩餘氣流51接著可驟沸於氣液分離器43中。在交叉交換器/冷卻器45、33中將來自分離器43之蒸氣加熱回35℃至45℃之溫度，且接著經由流動管線55遞送至膜分離單元24。來自膜分離單元24之富含氫氣之滲透物7隨後經壓縮且再循環返回至PSA單元22以用於額外氫氣回收，同時滯留物6作為系統尾氣遞送至燃料氣頭。
雖然圖3說明二個交叉交換器33、45及二個氣液分離器37、43，但可視自PSA單元純化剩餘氣體4中之H2之需要或基於對將饋料55中之H2濃縮至膜分離單元24之需要而利用低溫下之額外交換器及分離器。
根據本文實施例，PSA、低溫分離及膜之組合可提供96%至99%範圍內之整體H2回收。
整合低溫分離(諸如在圖3之實施例中)可冷凝重烴，而輕餾分(包括氫氣及存在於製程氣體或廢氣中之其他不可冷凝組分)可在膜系統中處理。此可能使得在膜單元中處理具有更高純度之饋料氣體流，其可能提供較佳的H2回收及純度。較高純度H2之益處亦可用於在較低壓力下操作膜系統。
對於所有此等組態，膜系統可為單級或多級系統，此取決於膜滲透物中H2純度及H2回收之要求。H2純度及跨膜回收影響整個膜整合之PSA系 統的H2整體回收率。
本文實施例亦可擴展至H2回收過程之其他模式。H2亦經由低溫分離回收，其中利用致冷劑回收H2。在此等實施例中，膜可用於增強H2回收，藉此減少致冷系統上之負載，從而產生過程之較佳經濟情況。
經由如圖2及圖3中所說明之過程產生之尾氣流7可如上文所提及用作燃料氣體或用於一些其他製程氣體。替代地，含有一氧化碳、二氧化碳或其他含碳分子之尾氣流可饋入至碳捕獲單元。由本文中所描述之方法產生的較高氫氣回收率可導致進入下游碳捕獲單元的尾氣量較少。此外，較低氫氣量或幾乎不存在氫氣亦有助於濃縮饋入至碳捕獲單元的二氧化碳，從而使脫碳更高效。較低濃度及量之氫氣亦可使得碳捕獲單元所需之過程單元尺寸較小，從而降低此類單元之資本成本。
如上文所描述，本文實施例利用PSA及/或低溫分離以及膜分離來改進混合氣流中的氫氣回收。藉由避免將高價值氫氣損失至低價值燃料氣體池中，經改進之氫氣回收將為相關工廠提供節約操作費用之益處。另外，此亦將幫助使得尾氣脫碳(自尾氣中捕獲碳)更高效且容量更小。
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當使用詞語「大約(approximately)」或「約(about)」時，此術語可意謂值之差異可能高達±10%、高達5%、高達2%、高達1%、高達0.5%、高達0.1%或高達0.01%。
範圍可表示為自約一個特定值至約另一特定值(包括端點)。當表述此類範圍時，應理解，另一實施例為一個特定值至另一個特定值，以及在該範圍內之所有特定值及其組合。
儘管本揭露內容包括有限數目個實施例，但受益於本揭露內容之熟習此項技術者應瞭解，可設計不脫離本揭露內容之範疇的其他實施例。因此，範疇應僅由所附申請專利範圍限制。
1:製程氣體或廢氣流，饋料流，流動料流
2:製程氣體或廢氣流，流動料流
3:氫氣產物，氫氣產物流
4:剩餘氣體，料流，流動料流，剩餘氣流，PSA尾氣，PSA尾氣流
5:剩餘氣體，料流，流動料流，剩餘氣流
6:尾氣流，滯留物
7:流動料流，氫氣滲透物，滲透物流，富含氫氣之滲透物流，富含氫氣之滲透物，尾氣流
8:滲透物流
22:PSA單元
24:膜分離系統，膜分離單元
26,28:壓縮機

Claims (13)

  1. 一種用於回收氫氣之方法，該方法包含：將包含氫氣及額外氣體之一氣流饋入至一變壓吸附系統；將包含氫氣之一膜滲透物流饋入至該變壓吸附系統；在該變壓吸附系統中，將一部分該氫氣與該等額外氣體分離以回收一氫氣產物流及包含未分離氫氣及該等額外氣體之一變壓吸附尾氣流；將該變壓吸附尾氣流饋入至一膜分離單元；在該膜分離單元中，將氫氣與該等額外氣體分離以回收(i)饋入至該變壓吸附系統之該包含氫氣之膜滲透物流及(ii)包含該等額外氣體之一膜尾氣流；及部分地冷凝該變壓吸附尾氣流，回收一PSA尾氣冷凝流及一PSA尾氣蒸氣流，且將該PSA尾氣蒸氣流作為饋入至該膜分離單元中之該變壓吸附尾氣流饋入。
  2. 如請求項1之方法，其進一步包含在該膜分離單元之上游壓縮該變壓吸附尾氣流。
  3. 如請求項1或請求項2之方法，其進一步包含在該變壓吸附系統之上游壓縮該膜滲透物流。
  4. 如請求項中1或請求項2之方法，其進一步包含部分地冷凝該氣流，回收一冷凝流及一蒸氣流，且將該蒸氣流作為饋入至該變壓吸附系統中之該氣流饋入。
  5. 如請求項1或請求項2之方法，其中該氣流在25至35巴表壓(barg)範圍內之壓力下饋入至該變壓吸附系統中。
  6. 如請求項1或請求項2之方法，其中該變壓吸附尾氣流在1至5巴表壓範圍內之壓力下自該變壓吸附系統回收且在饋入至該膜分離單元之前壓縮至10至20巴表壓之壓力。
  7. 如請求項1或請求項2之方法，其中該膜滲透物流在1至2巴表壓範圍內之壓力下自該膜分離單元回收且壓縮至在25至35巴表壓範圍內之壓力以用於饋入至該變壓吸附系統。
  8. 如請求項1或請求項2之方法，其中該膜尾氣流在8至18巴表壓範圍內之壓力下回收。
  9. 一種用於回收氫氣之系統，該系統包含：一用於將包含氫氣及額外氣體之一氣流饋入至一變壓吸附系統的流動管線；一用於將包含氫氣之一膜滲透物流饋入至該變壓吸附系統的流動管線；該變壓吸附系統，其經組態以用於將一部分該氫氣與該等額外氣體分離以回收一氫氣產物流及包含未分離氫氣及該等額外氣體之一變壓吸附尾氣流；一用於將該變壓吸附尾氣流饋入至一膜分離單元的流動管線；該膜分離單元，其經組態以用於將氫氣與該等額外氣體分離以回收(i)饋入至該變壓吸附系統之該包含氫氣之膜滲透物流及(ii)包含該等額外氣體之一膜尾氣流；及一致冷/分離系統，該致冷/分離系統經組態以用於部分地冷凝該變壓吸附尾氣流，回收一PSA尾氣冷凝流及一PSA尾氣蒸氣流，且將該PSA尾氣蒸氣流作為饋入至該膜分離單元中之該變壓吸附尾氣流饋入。
  10. 如請求項9之系統，其進一步包含一壓縮機，該壓縮機用於在該膜分離單元之上游壓縮該變壓吸附尾氣流。
  11. 如請求項9或請求項10之系統，其進一步包含一壓縮機，該壓縮機用於在該變壓吸附系統之上游壓縮該膜滲透物流。
  12. 如請求項9或請求項10之系統，其進一步包含一致冷/分離系統，該致冷/分離系統用於部分地冷凝該氣流，回收一冷凝流及一蒸氣流；以及 一用於將該蒸氣流作為饋入至該變壓吸附系統中之該氣流饋入的流動管線。
  13. 如請求項9之系統，該致冷/分離系統包含：一交叉交換器，其經組態以在該氣流、該變壓吸附尾氣流、該蒸氣流、該PSA尾氣蒸氣流、該冷凝流與該PSA尾氣冷凝流之混合物及一致冷劑之間交換熱量，從而產生部分冷凝之一氣流；一交叉交換器，其經組態以在該變壓吸附尾氣流與該PSA尾氣蒸氣流之間交換熱量，從而產生部分冷凝之一變壓吸附尾氣流；一氣液分離器，其經組態以接收該部分冷凝之氣流，該氣液分離器包括用於回收該蒸氣流之一蒸氣出口及用於回收該冷凝流之一液體出口；及一第二氣液分離器，其經組態以接收該部分冷凝之變壓吸附尾氣流，該第二氣液分離器包括用於回收該PSA尾氣蒸氣流之一蒸氣出口及用於回收該PSA尾氣冷凝流之一液體出口。
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