CN105431221A - 通过从soec产生的co的膜纯化制备高纯度co的方法 - Google Patents
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Abstract
本发明涉及一种通过在固态氧化物电解池(solid?oxide?electrolysis?cell,SOEC)中产生的CO的膜纯化制备高纯度一氧化碳(CO)的方法,其包含以下步骤:通过CO2的SOEC电解生成CO与CO2的气体混合物,经由压缩器或喷射器施加适度压力于一或多个连接至该SOEC的出口的膜单元中的膜的滞留侧上,将比该适度压力低的压力施加于该膜的渗透侧上,将现在富含CO的滞留物流分成两个单独的部分,使该滞留物流的第一部分膨胀以达到渗透低压条件,引导该滞留物的上述部分至该膜的渗透侧以降低此侧上的CO2的分压,及再循环出口渗透物流返回至该SOEC与新制CO2一起作为进料气体。该膜单元优选地经设计成具有管状膜或多个串联连接的平面膜,且该滞留物流与该渗透物流以逆流模式运行。
Description
技术领域
本发明涉及一种通过在固态氧化物电解池(solidoxideelectrolysiscell,SOEC)中产生的CO的膜纯化制备高纯度一氧化碳(CO)的方法。
背景技术
固态氧化物电解池为以逆向模式运行的固态氧化物燃料电池(solidoxidefuelcell,SOFC),其使用固态氧化物或陶瓷电解质通过电解水来制备例如氧气与氢气。其亦可用于自二氧化碳(CO2)制备CO,伴以施加的电流将二氧化碳引向SOEC或SOEC堆的燃料侧。将过量氧气传输至SOEC的氧气侧,任选地使用空气、氮气或CO2冲洗氧气侧,且然后使来自SOEC的含有与CO2混合的CO的产物流经历分离过程。
高纯度一氧化碳为合成化学物质的重要原料。大部分合成化学物质的反应要求高温以及高压,且因此所用CO应具有可能的最低含量的二氧化碳(CO2),该二氧化碳通过氧化而腐蚀反应器。另外,CO2会限制所产生的CO所参与的反应的平衡转化率。CO2还可以抑制使用CO的反应的动力学。
高纯度CO的制备描述于多个专利公开案中。由此,US5,482,539描述一种多阶段半透膜方法及用于气体分离的设备。然而,此专利并不涉及在电解池中产生的CO。
US6,787,118涉及CO的选择性移除。更具体地,其涉及催化剂组合物,该等催化剂组合物适用于在低温下破坏含氧气体流中的挥发性有机碳化合物(volatileorganiccarboncompound,VOC)及适用于自含氢气体选择性氧化一氧化碳。此专利不涉及任何膜的使用。
US2009/0014336涉及将二氧化碳在水性介质中电解成一氧化碳与氢气以便制备甲醇。然而,此专利申请案既不涉及使用SOEC制备CO亦未涉及膜的使用。
在US5,814,127中揭示一种系统,其中膜单元耦接至电解池的出口。此专利涉及在铝电解池中制备铝且随后在膜单元中自排出气体移除无机氟化物,其中将气体分成富含氟化物的滞留物流与缺乏氟化物的渗透物流。此与CO的纯化无关,但该系统类似本发明中所使用的系统。
最后,EP0129444与US4,539,020涉及通过变压吸附(pressureswingadsorption,PSA)获得的高纯度CO。
实际上,变压吸附(PSA)为能够以经济可行的方式以适用于“小规模CO”,亦即CO产量为1Nm3/h至200Nm3/h的规模自CO与CO2的混合物纯化CO至95%及95%以上的纯度的唯一已知技术。仅仅极有限数目的生产者能够供应在此规模的PSA单元。此外,PSA单元向较小单元增添相当大的复杂度与成本。出于此等原因,需要寻找PSA的可行的替代方案用于以小规模纯化所产生的CO。
自SOEC下游安装膜分离单元为PSA的有吸引力的替代方案,主要归因于其简单性,因为膜分离单元操作无需任何移动部件,但亦归因于减少资金支出(capitalexpenditure,CAPEX),因为其模组性质。
气体分离膜目前用于自天然气与合成气移除CO2。此类膜可基于聚合物或沸石,涂布于氧化铝管上的,且其一般具有针对通过膜传输CO2的选择性,而将烃、H2与CO阻止在滞留侧上。CO/CO2的典型选择性常数在5与20之间,且通量可在每平方米膜面积20Nm3/h至200Nm3/h内变化。
通过分压的差值驱动膜分离,且因此其最适合于移除诸如CO2的大多数杂质,但当用于分离的驱动力降低时需要大量的膜面积以达到高纯度。
所有对于CO与对于CO2在渗透性方面具有差异的膜,其中相比于对于CO,对于CO2的膜渗透性更高,可用于本发明。陶瓷膜、经涂布的陶瓷膜与聚合物膜满足此等准则。膜可具有平面或管状形状,且其可以单个膜单元或以多个串联或并联的膜单元形式使用。
可通过施加高绝对压力于膜的滞留侧上且施加近似真空于膜的渗透侧上来增强用于分离的驱动力。然而,实务上对于安装多阶段压缩器以达到高压及驱动压缩器所需的功率而言存在CAPEX限制。最大压力差亦受膜及膜模组的机械强度限制。
发明内容
本发明涉及自CO与CO2的混合物选择性分离CO,尤其涉及通过SOEC电解小规模制备CO。原理与蒸馏中的回流塔非常类似。
更具体地,本发明涉及一种通过固态氧化物电解池(SOEC)中产生的CO的膜纯化制备高纯度一氧化碳(CO)的方法,该方法包含以下步骤:
(1)通过CO2的SOEC电解生成CO与CO2的气体混合物,
(2)经由压缩器或喷射器施加适度压力于连接至SOEC的出口的膜单元中的膜的滞留侧上,
(3)将比步骤(2)中的压力低的压力施加于膜的渗透侧上,
(4)将现在富含CO的滞留物流分成两个单独的部分,
(5)使滞留物流的第一部分膨胀以达到渗透低压条件,
(6)引导滞留物的上述部分至膜的渗透侧以降低此侧上的CO2的分压,及
(7)再循环出口渗透物流返回至SOEC与新制CO2一起作为进料气体。
附图说明
图1显示固态氧化物电解池(SOEC)单元。
具体实施方式
在上述步骤(6)中通过降低膜的渗透侧上的CO2的分压,使CO2流过膜的驱动力增加。另外,降低CO传输通过膜的驱动力,且由此当目标为高纯度的CO时可增加CO的产率。在上述步骤(7)中完全或部分再循环出口渗透物流返回至SOEC与新制CO2一起作为进料气体,从而提高CO2产率。
涉及膜的滞留侧上的适度压力,其可自250巴表压下至3巴表压,优选地自175巴表压下至3巴表压,更优选地自40巴表压下至3巴表压,且最优选地自20巴表压下至5巴表压。
膜的渗透侧上的较低压力可在-0.8巴表压与50巴表压之间,优选地在-0.8巴表压与10巴表压之间,更优选地在-0.8巴表压与3巴表压之间,甚至更优选地在-0.8巴表压与2巴表压之间,且最优选地在-0.3巴表压与0.5巴表压之间,尤其在0与0.3巴表压之间。
涉及如上文所提及的与蒸馏的类比,将滞留物流分成两个单独部分亦类似于在蒸馏塔的顶部处的回流。另外,SOEC单元具有与蒸馏单元中的再沸器类似的功能;参见附图1。
膜单元优选地经设计成具有管状膜或多个串联连接的平面膜,其中滞留物流与渗透物流以逆流模式运行。此意味着来自滞留侧的富含CO的回流流进入(在膨胀之后)膜单元的渗透侧,在相对端,进料气体自SOEC单元进入膜单元。
可参见图1进一步概述根据本发明的方法,其显示固态氧化物电解池(SOEC)单元,其中氧气侧处于顶部、电解质处于中间且燃料侧处于底部。伴以施加的电流将CO2引向SOEC单元的燃料侧,以将CO2转化成CO,且传输任何过剩的氧气至SOEC单元的氧气侧。将CO2亦引向氧气侧以冲洗此侧,但空气或氮气亦可用于此目的。冲洗SOEC单元的氧气侧具有两个优势,更具体地(1)降低氧气浓度与相关的腐蚀效应及(2)提供向SOEC单元(其运行为吸热的)中馈入能量的方式。
来自SOEC的产物流含有混合的CO与CO2,将其引向用以于膜的滞留侧上产生高绝对压力的压缩器C。通过引导CO产物流的一部分通过减压阀门P且进入膜的渗透侧来施加较低压力于膜的渗透侧上。
Claims (8)
1.一种通过在固态氧化物电解池(solidoxideelectrolysiscell,SOEC)中产生的CO的膜纯化制备高纯度一氧化碳(CO)的方法,该方法包含以下步骤:
(1)通过CO2的SOEC电解生成CO与CO2的气体混合物,
(2)经由压缩器或喷射器施加适度压力于一或多个连接至该SOEC的出口的膜单元中的膜的滞留侧上,
(3)将比步骤(2)中的压力低的压力施加于该膜的渗透侧上,
(4)将现在富含CO的滞留物流分成两个单独的部分,
(5)使该滞留物流的第一部分膨胀以达到渗透低压条件,
(6)引导该滞留物的上述部分至该膜的渗透侧以降低此侧上的CO2的分压,及
(7)再循环出口渗透物流返回至该SOEC与新制CO2一起作为进料气体。
2.如权利要求1的方法,其中该膜选自由陶瓷膜、经涂布的陶瓷膜(诸如经沸石涂布的膜)及聚合物膜组成的组。
3.如权利要求1或2的方法,其中该膜单元经设计成具有管状膜或多个串联连接的平面膜,且其中该滞留物流与该渗透物流以逆流模式运行。
4.如权利要求1至3中任一项的方法,其中步骤(2)中的该适度压力为自250巴表压下至3巴表压,优选地自175巴表压下至3巴表压。
5.如权利要求4的方法,其中步骤(2)中的该适度压力为自40巴表压下至3巴表压,且优选地自20巴表压下至5巴表压。
6.如权利要求1至3中任一项的方法,其中步骤(3)中的该较低压力在-0.8巴表压与50巴表压之间,优选地在-0.8巴表压与10巴表压之间。
7.如权利要求6的方法,其中步骤(3)中的该较低压力在-0.8巴表压与3巴表压之间,优选地在-0.8巴表压与2巴表压之间。
8.如权利要求7的方法,其中步骤(3)中的该较低压力在-0.3巴表压与0.5巴表压之间,优选地在0与0.3巴表压之间。
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EP13178475.3 | 2013-07-30 | ||
EP13178475.3A EP2832421B1 (en) | 2013-07-30 | 2013-07-30 | Process for producing high purity co by membrane purification of soec-produced co |
PCT/EP2014/062362 WO2015014527A1 (en) | 2013-07-30 | 2014-06-13 | Process for producing high purity co by membrane purification of soec-produced co |
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CN105431221A true CN105431221A (zh) | 2016-03-23 |
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US (1) | US20160151739A1 (zh) |
EP (1) | EP2832421B1 (zh) |
CN (1) | CN105431221A (zh) |
AR (1) | AR097092A1 (zh) |
CA (1) | CA2916959A1 (zh) |
ES (1) | ES2583903T3 (zh) |
TW (1) | TW201516184A (zh) |
WO (1) | WO2015014527A1 (zh) |
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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 |
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DE102018000214A1 (de) | 2018-01-12 | 2019-07-18 | Linde Aktiengesellschaft | Herstellung eines zumindest Kohlenmonoxid enthaltenden Gasprodukts |
DE102018000213A1 (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 |
DE102018202335A1 (de) * | 2018-02-15 | 2019-08-22 | Linde Aktiengesellschaft | Anlage zur elektrochemischen Herstellung eines CO-haltigen Gasprodukts |
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DE102018003343A1 (de) | 2018-04-24 | 2019-10-24 | Linde Aktiengesellschaft | Verfahren und Anlage zur Herstellung von Ethanol |
DE102018003342A1 (de) | 2018-04-24 | 2019-10-24 | Linde Aktiengesellschaft | Herstellung eines zumindest Kohlenmonoxid enthaltenden Gasprodukts |
DE102018003332A1 (de) | 2018-04-24 | 2019-10-24 | Linde Aktiengesellschaft | Herstellung eines Syntheseprodukts |
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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 |
US20240035169A1 (en) | 2020-12-22 | 2024-02-01 | Topsoe A/S | An improved method for operation of a solid oxide electrolysis cell in carbon dioxide electrolysis |
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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ES2583903T3 (es) | 2016-09-22 |
EP2832421B1 (en) | 2016-05-25 |
CA2916959A1 (en) | 2015-02-05 |
TW201516184A (zh) | 2015-05-01 |
US20160151739A1 (en) | 2016-06-02 |
AR097092A1 (es) | 2016-02-17 |
EP2832421A1 (en) | 2015-02-04 |
WO2015014527A1 (en) | 2015-02-05 |
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