TW201516184A - 藉由從ｓｏｅｃ產生之ｃｏ的膜純化製備高純度ｃｏ的方法 - Google Patents
藉由從ｓｏｅｃ產生之ｃｏ的膜純化製備高純度ｃｏ的方法 Download PDFInfo
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- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 1
- 239000012736 aqueous medium Substances 0.000 description 1
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- 229910052757 nitrogen Inorganic materials 0.000 description 1
- MWUXSHHQAYIFBG-UHFFFAOYSA-N nitrogen oxide Inorganic materials O=[N] MWUXSHHQAYIFBG-UHFFFAOYSA-N 0.000 description 1
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Abstract
本發明係關於一種藉由在固態氧化物電解池(solid oxide electrolysis cell，SOEC)中產生之CO的膜純化製備高純度一氧化碳(CO)之方法，其包含以下步驟：藉由CO2之SOEC電解生成CO與CO2之氣體混合物，經由壓縮器或噴射器施加適度壓力於一或多個連接至該SOEC之出口之膜單元中的膜之滯留側上，將比該適度壓力低的壓力施加於該膜之滲透側上，將現在富含CO之滯留物流分成兩個單獨的部分，使該滯留物流之第一部分膨脹以達到滲透低壓條件，引導該滯留物之上述部分至該膜之滲透側以降低此側上的CO2之分壓，及再循環出口滲透物流返回至該SOEC與新製CO2一起作為饋入氣體。
該膜單元較佳地經設計成具有管狀膜或多個串聯連接的平面膜，且該滯留物流與該滲透物流以逆流模式運行。
Description
本發明係關於一種藉由在固態氧化物電解池(solid oxide electrolysis cell，SOEC)中產生之CO的膜純化製備高純度一氧化碳(CO)的方法。
固態氧化物電解池為以逆向模式運行的固態氧化物燃料電池(solid oxide fuel cell，SOFC)，其使用固態氧化物或陶瓷電解質藉由電解水來製備例如氧氣與氫氣。其亦可用於自二氧化碳(CO2)製備CO，伴以施加的電流將二氧化碳引向SOEC或SOEC堆疊之燃料側。將過量氧氣傳輸至SOEC之氧氣側，視情況使用空氣、氮氣或CO2沖洗氧氣側，且然後使來自SOEC之含有與CO2混合之CO的產物流經歷分離製程。
高純度一氧化碳為合成化學物質之重要原料。大部分合成化學物質之反應要求高溫以及高壓，且因此所用CO應具有可能的最低含量之二氧化碳(CO2)，該二氧化碳藉由氧化而腐蝕反應器。另外，CO2會限制所產生的CO所參與的反應之平衡轉化率。CO2亦會抑制使用CO之反應的動力學。
高純度CO之製備描述於多個專利公開案中。由此，US 5,482,539描述一種多階段半透膜方法及用於氣體分離之設備。然而，此專利並不涉及在電解池中產生的CO。
US 6,787,118係關於CO之選擇性移除。更特定言之，其涉
及催化劑組合物，該等催化劑組合物適用於在低溫下破壞含氧氣體流中之揮發性有機碳化合物(volatile organic carbon compound，VOC)及適用於自含氫氣體選擇性氧化一氧化碳。此專利不關於任何膜之使用。
US 2009/0014336係關於將二氧化碳在水性介質中電解成一
氧化碳與氫氣以便製備甲醇。然而，此專利申請案既不關於使用SOEC製備CO亦未關於膜之使用。
在US 5,814,127中揭示一種系統，其中膜單元耦接至電解池
之出口。此專利係關於在鋁電解池中製備鋁且隨後在膜單元中自排出氣體移除無機氟化物，其中將氣體分成富含氟化物的滯留物流與缺乏氟化物的滲透物流。此與CO之純化無關，但該系統類似本發明中所使用之系統。
最後，EP 0 129 444與US 4,539,020係關於藉由變壓吸附
(pressure swing adsorption，PSA)獲得之高純度CO。
實際上，變壓吸附(PSA)為能夠以經濟可行的方式以適用
於「小規模CO」，亦即CO產量為1Nm3/h至200Nm3/h之規模自CO與CO2之混合物純化CO至95%及95%以上之純度的唯一已知技術。僅僅極有限數目之生產者能夠供應在此規模之PSA單元。此外，PSA單元向較小單元增添相當大的複雜度與成本。出於此等原因，需要尋找PSA之可行的替代方案用於以小規模純化所產生的CO。
自SOEC下游安裝膜分離單元為PSA之有吸引力的替代方
案，主要歸因於其簡單性，因為膜分離單元操作無需任何移動部件，但亦歸因於減少資金支出(capital expenditure，CAPEX)，因為其模組性質。
氣體分離膜目前用於自天然氣與合成氣移除CO2。此類膜可
基於塗佈於氧化鋁管上的聚合物或沸石，且其一般具有針對通過膜傳輸CO2之選擇性，而將烴、H2與CO阻止在滯留側上。CO/CO2之典型選擇性常數
在5與20之間，且通量可在每平方公尺膜面積20Nm3/h至200Nm3/h內變化。
藉由分壓的差值驅動膜分離，且因此其最適合於移除諸如
CO2之大多數雜質，但當用於分離之驅動力降低時需要大量的膜面積以達到高純度。
所有對於CO與對於CO2在滲透性方面具有差異的膜(其中
CO2之膜滲透性高於CO之膜滲透性)可用於本發明。陶瓷膜、經塗佈之陶瓷膜與聚合物膜滿足此等準則。膜可具有平面或管狀形狀，且其可以單個膜單元或以多個串聯或並聯之膜單元形式使用。
可藉由施加高絕對壓力於膜之滯留側上且施加近似真空於
膜之滲透側上來增強用於分離之驅動力。然而，實務上對於安裝多階段壓縮器以達到高壓及驅動壓縮器所需的功率而言存在CAPEX限制。最大壓力差亦受膜及膜模組之機械強度限制。
本發明係關於自CO與CO2之混合物選擇性分離CO，尤其關於藉由SOEC電解小規模製備CO。原理與蒸餾中之回流塔非常類似。
更特定言之，本發明關於一種藉由固態氧化物電解池(SOEC)中產生的CO之膜純化製備高純度一氧化碳(CO)的方法，該方法包含以下步驟：(1)藉由CO2之SOEC電解生成CO與CO2之氣體混合物，(2)經由壓縮器或噴射器施加適度壓力於連接至SOEC之出口之膜單元中的膜之滯留側上，(3)將比步驟(2)中之壓力低的壓力施加於膜之滲透側上，(4)將現在富含CO之滯留物流分成兩個單獨的部分，(5)使滯留物流之第一部分膨脹以達到滲透低壓條件，
(6)引導滯留物之上述部分至膜之滲透側以降低此側上的CO2之分壓，及(7)再循環出口滲透物流返回至SOEC與新製CO2一起作為饋入氣體。
在上述步驟(6)中藉由降低膜之滲透側上的CO2之分壓，使CO2流過膜之驅動力增加。另外，降低CO傳輸通過膜之驅動力，且由此當目標為高純度之CO時可增加CO之產率。在上述步驟(7)中完全或部分再循環出口滲透物流返回至SOEC與新製CO2一起作為饋入氣體，從而提高CO2產率。
關於膜之滯留側上的適度壓力，其可自250巴錶壓下至3巴錶壓，較佳地自175巴錶壓下至3 barg，更佳地自40巴錶壓下至3巴錶壓，且最佳地自20巴錶壓下至5巴錶壓。
膜之滲透側上的較低壓力可在-0.8巴錶壓與50巴錶壓之間，較佳地在-0.8巴錶壓與10巴錶壓之間，更佳地在-0.8巴錶壓與3巴錶壓之間，甚至更佳地在-0.8巴錶壓與2巴錶壓之間，且最佳地在-0.3巴錶壓與0.5巴錶壓之間，尤其在0與0.3巴錶壓之間。
關於如上文所提及之與蒸餾之類比，將滯留物流分成兩個單獨部分亦類似於在蒸餾塔之頂部處的回流。另外，SOEC單元具有與蒸餾單元中的再沸器類似的功能；參見附圖1。
膜單元較佳地經設計成具有管狀膜或多個串聯連接的平面膜，其中滯留物流與滲透物流以逆流模式運行。此意味著來自滯留側之富含CO的回流流進入(在膨脹之後)膜單元之滲透側，在相對端，來自饋入氣體之富含CO的回流流自SOEC單元進入膜單元。
可參見圖1進一步概述根據本發明之方法，其顯示固態氧化
物電解池(SOEC)單元，其中氧氣側處於頂部、電解質處於中間且燃料側處於底部。伴以施加的電流將CO2引向SOEC單元之燃料側，以將CO2轉化成CO，且傳輸任何過剩的氧氣至SOEC單元之氧氣側。將CO2亦引向氧氣側以沖洗此側，但空氣或氮氣亦可用於此目的。沖洗SOEC單元之氧氣側具有兩個優勢，更特定言之(1)降低氧氣濃度與相關的腐蝕效應及(2)提供向SOEC單元(其運行為吸熱的)中饋入能量之方式。
來自SOEC之產物流含有混合的CO與CO2，將其引向用以
於膜之滯留側上產生高絕對壓力的壓縮器C。藉由引導CO產物流之一部分通過減壓閥門P且進入膜之滲透側來施加較低壓力於膜之滲透側上。
Claims (8)
- 一種藉由在固態氧化物電解池(solid oxide electrolysis cell，SOEC)中產生之CO的膜純化製備高純度一氧化碳(CO)之方法，該方法包含以下步驟：(1)藉由CO2之SOEC電解生成CO與CO2之氣體混合物，(2)經由壓縮器或噴射器施加適度壓力於一或多個連接至該SOEC之出口之膜單元中的膜之滯留側上，(3)將比步驟(2)中之壓力低的壓力施加於該膜之滲透側上，(4)將現在富含CO之滯留物流分成兩個單獨的部分，(5)使該滯留物流之第一部分膨脹以達到滲透低壓條件，(6)引導該滯留物之上述部分至該膜之滲透側以降低此側上的CO2之分壓，及(7)再循環出口滲透物流返回至該SOEC與新製CO2一起作為饋入氣體。
- 如申請專利範圍第1項之方法，其中該膜係選自由陶瓷膜、經塗佈之陶瓷膜(諸如經沸石塗佈之膜)及聚合物膜組成之群。
- 如申請專利範圍第1項或第2項之方法，其中該膜單元經設計成具有管狀膜或多個串聯連接的平面膜，且其中該滯留物流與該滲透物流以逆流模式運行。
- 如申請專利範圍第1項至第3項中任一項之方法，其中步驟(2)中的該適度壓力為自250巴錶壓下至3巴錶壓，較佳地自175巴錶壓下至3巴錶壓。
- 如申請專利範圍第4項之方法，其中步驟(2)中的該適度壓力為自40巴錶壓下至3巴錶壓，且較佳地自20巴錶壓下至5巴錶壓。
- 如申請專利範圍第1項至第3項中任一項之方法，其中步驟(3)中的該較低壓力在-0.8巴錶壓與50巴錶壓之間，較佳地在-0.8巴錶壓與10 巴錶壓之間。
- 如申請專利範圍第6項之方法，其中步驟(3)中的該較低壓力在-0.8巴錶壓與3巴錶壓之間，較佳地在-0.8巴錶壓與2巴錶壓之間。
- 如申請專利範圍第7項之方法，其中步驟(3)中的該較低壓力在-0.3巴錶壓與0.5巴錶壓之間，較佳地在0與0.3巴錶壓之間。
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| EP13178475.3A EP2832421B1 (en) | 2013-07-30 | 2013-07-30 | Process for producing high purity co by membrane purification of soec-produced co |
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| CN (1) | CN105431221A (zh) |
| AR (1) | AR097092A1 (zh) |
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| ES (1) | ES2583903T3 (zh) |
| TW (1) | TW201516184A (zh) |
| WO (1) | WO2015014527A1 (zh) |
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| DE102015202117A1 (de) | 2015-02-06 | 2016-08-11 | Siemens Aktiengesellschaft | Verfahren und Elektrolysesystem zur Kohlenstoffdioxid-Verwertung |
| DE102015202789A1 (de) * | 2015-02-17 | 2016-08-18 | Robert Bosch Gmbh | Produktgasaufbereitungsvorrichtung und Verfahren zum Aufbereiten eines Produktgases |
| ITUA20163761A1 (it) * | 2016-05-24 | 2017-11-24 | Microprogel S R L | Essicatore per gas |
| FR3063437B1 (fr) * | 2017-03-02 | 2019-03-29 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Installation et procede pour le traitement par permeation membranaire d'un flux gazeux d'alimentation comprenant du methane et du dioxyde de carbone |
| DE102017005680A1 (de) | 2017-06-14 | 2018-12-20 | Linde Aktiengesellschaft | Verfahren und Anlage zur Herstellung eines Kohlenmonoxid enthaltenden Gasprodukts |
| DE102017005681A1 (de) | 2017-06-14 | 2018-12-20 | Linde Aktiengesellschaft | Verfahren und Anlage zur Herstellung eines Kohlenmonoxid enthaltenden Gasprodukts |
| DE102017005678A1 (de) | 2017-06-14 | 2018-12-20 | Linde Aktiengesellschaft | Verfahren und Anlage zur Herstellung eines Kohlenmonoxid enthaltenden Gasprodukts |
| DE102018000213A1 (de) | 2018-01-12 | 2019-07-18 | Linde Aktiengesellschaft | Herstellung eines zumindest Kohlenmonoxid enthaltenden Gasprodukts |
| DE102018000214A1 (de) | 2018-01-12 | 2019-07-18 | Linde Aktiengesellschaft | Herstellung eines zumindest Kohlenmonoxid enthaltenden Gasprodukts |
| DE102018202344A1 (de) | 2018-02-15 | 2019-08-22 | Siemens Aktiengesellschaft | Elektrochemische Herstellung von Kohlenstoffmonoxid und/oder Synthesegas |
| DE102018202337A1 (de) | 2018-02-15 | 2019-08-22 | Linde Aktiengesellschaft | Elektrochemische Herstellung eines Gases umfassend CO mit Zwischenkühlung des Elektrolytstroms |
| DE102018202335A1 (de) | 2018-02-15 | 2019-08-22 | Linde Aktiengesellschaft | Anlage zur elektrochemischen Herstellung eines CO-haltigen Gasprodukts |
| DE102018003332A1 (de) | 2018-04-24 | 2019-10-24 | Linde Aktiengesellschaft | Herstellung eines Syntheseprodukts |
| DE102018003342A1 (de) | 2018-04-24 | 2019-10-24 | Linde Aktiengesellschaft | Herstellung eines zumindest Kohlenmonoxid enthaltenden Gasprodukts |
| DE102018003343A1 (de) | 2018-04-24 | 2019-10-24 | Linde Aktiengesellschaft | Verfahren und Anlage zur Herstellung von Ethanol |
| EP3574991A1 (en) | 2018-05-31 | 2019-12-04 | Haldor Topsøe A/S | Steam reforming heated by resistance heating |
| DE102018009198A1 (de) * | 2018-11-22 | 2020-05-28 | Linde Aktiengesellschaft | Verfahren zum Wechsel der Betriebsweise einer Elektrolyseanlage sowie Elektrolyseanlage |
| DE102019007265A1 (de) | 2019-10-18 | 2021-04-22 | Linde Gmbh | Verfahren und Anlage zur Herstellung eines an Kohlenstoffmonoxid reichen Gasprodukts |
| DE102020000476A1 (de) | 2020-01-27 | 2021-07-29 | Linde Gmbh | Verfahren und Anlage zur Herstellung von Wasserstoff |
| DE102020000937A1 (de) | 2020-02-14 | 2021-08-19 | Linde Gmbh | Verfahren und Anlage zur Bereitstellung eines Industrieprodukts unter Verwendung von Sauerstoff |
| JP2023531388A (ja) * | 2020-06-09 | 2023-07-24 | トゥエルブ ベネフィット コーポレーション | 電解槽出力における高濃度の多電子生成物またはｃｏのためのシステムおよび方法 |
| KR20230123934A (ko) | 2020-12-22 | 2023-08-24 | 토프쉐 에이/에스 | 이산화탄소 전기분해에서 고체 산화물 전기분해 전지의 개선된 작동 방법 |
| EP4324957A1 (de) | 2022-08-19 | 2024-02-21 | Linde GmbH | Verfahren und anlage zur herstellung eines wasserstoff enthaltenden produkts |
| EP4345191A1 (de) | 2022-09-30 | 2024-04-03 | Linde GmbH | Verfahren und anlage zur herstellung eines wasserstoff enthaltend en produkts unter einsatz einer elektrolyse |
| EP4345086A1 (de) | 2022-09-30 | 2024-04-03 | Linde GmbH | Verfahren und anlage zur herstellung von methanol |
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| EP0129444B2 (en) | 1983-06-20 | 1995-04-19 | Kawasaki Steel Corporation | Methods for obtaining high-purity carbon monoxide |
| US4539020A (en) | 1983-07-10 | 1985-09-03 | Kawasaki Steel Corporation | Methods for obtaining high-purity carbon monoxide |
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| US5814127A (en) | 1996-12-23 | 1998-09-29 | American Air Liquide Inc. | Process for recovering CF4 and C2 F6 from a gas |
| WO2000068146A1 (en) * | 1999-05-06 | 2000-11-16 | L'air Liquide Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | On site carbon monoxide generator |
| WO2001045833A1 (en) | 1999-12-20 | 2001-06-28 | Eltron Research, Inc. | CATALYSTS AND METHODS FOR LOW-TEMPERATURE DESTRUCTION OF VOCs IN AIR AND SELECTIVE REMOVAL OF CO |
| KR20100036317A (ko) * | 2007-07-13 | 2010-04-07 | 유니버시티 오브 써던 캘리포니아 | 메탄올을 제조하기 위해 수성 매질의 이산화탄소를 일산화탄소와 수소로 전기분해하는 방법 |
| US8591718B2 (en) * | 2010-04-19 | 2013-11-26 | Praxair Technology, Inc. | Electrochemical carbon monoxide production |
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2013
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- 2014-06-13 US US14/903,186 patent/US20160151739A1/en not_active Abandoned
- 2014-06-17 TW TW103120810A patent/TW201516184A/zh unknown
- 2014-07-28 AR ARP140102804A patent/AR097092A1/es unknown
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| CN105431221A (zh) | 2016-03-23 |
| ES2583903T3 (es) | 2016-09-22 |
| EP2832421A1 (en) | 2015-02-04 |
| CA2916959A1 (en) | 2015-02-05 |
| AR097092A1 (es) | 2016-02-17 |
| WO2015014527A1 (en) | 2015-02-05 |
| EP2832421B1 (en) | 2016-05-25 |
| US20160151739A1 (en) | 2016-06-02 |
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