CN102083513A - 用于从烟道气流中去除co2的助催化剂增强的基于冷冻氨的系统和方法 - Google Patents
用于从烟道气流中去除co2的助催化剂增强的基于冷冻氨的系统和方法 Download PDFInfo
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Abstract
提供一种基于冷冻氨的CO2捕获系统和方法。用助催化剂帮助加速某些与基于冷冻氨的离子溶液与含CO2气流的接触基本上同时发生的和/或由该接触导致的捕获反应。助催化剂可以是哌嗪或酶体系。
Description
技术领域
本发明涉及从包含二氧化碳和二氧化硫的工艺流程气体中去除二氧化碳(CO2)的系统和方法。更特别地,本发明针对的是用于去除烟道气流中的CO2的一种基于冷冻氨的烟道气处理系统。本发明使包含助催化剂的离子溶液与烟道气接触。
相关申请的交叉引用
本申请要求共同未决的美国临时申请“EnhancedCO2Absorption in a ChilledAmmonia Based Post-Combustion Flue Gas Processing System”的优先权,该申请的序列号为US 60/992,340,申请日为12/05/2007,其公开的内容全部引入本文作为参考。
发明内容
本发明的实施方案提供了一种从工艺流程气流中捕获二氧化碳(CO2)的系统和方法。在系统结构上,尤其可以实施该系统的一个实施方案使得包括设计用于接收烟道气流的吸收容器;进一步设计用于接收吸收剂溶液供给的吸收容器。该吸收容器包括气液传质装置(MTD),其设计用于使烟道气流与吸收剂溶液接触。
本发明的实施方案还可以看作是提供一种从烟道气流中去除CO2的方法。关于这点,此类方法的其中一个实施方案尤其可以大体概括为以下步骤:使助催化剂与吸收剂离子溶液(离子溶液)相组合;使组合后的助催化剂和离子溶液与包含CO2的烟道气流接触;和,使组合后的的助催化剂和离子溶液再生,从而释放从烟道气中吸收的CO2。
本发明的其它系统、方法、特点和优点对于本领域普通技术人员一旦查看下面的图和具体描述变得显而易见的。理解的是,所有附加的系统、方法、特点和优点包括在本发明书中、在本发明的范围内,受到附随的权利要求书保护。
背景技术
当在燃烧设备(如向发电厂提供蒸汽的锅炉系统)中的燃料如煤、石油、泥炭、废物等燃烧时,产生了热工艺流程气体(或烟道气)。尤其,这样的烟道气通常包括二氧化碳(CO2)。二氧化碳释放到大气层中对环境的负面影响已经被广泛认知,并引起了开发适合于从上述燃料燃烧中产生的热工艺流程气体中去除二氧化碳工艺方法。这样的一种系统和方法先前已经被公开,并涉及用于从燃烧后烟道气流中去除二氧化碳(CO2)的单级基于冷冻氨的系统和方法。
已知的基于冷冻氨的系统和工艺(CAP)提供了一种用于从气流例如燃烧后的烟道气流中捕获/去除CO2的相对低成本的装置。这样的系统和工艺的例子已经先前被未决专利申请PCT/US2005/012794(国际公开号:WO 2006/022885,发明人:EIi Gal)公开,其申请日为2005年4月12日,发明名称为“Ultra Cleaningof Combustion Gas Including the Removal ofCO2”。该工艺中,通过使冷冻氨的离子溶液(或浆液)与含CO2的烟道气流接触来实现从烟道气流中吸收CO2。
图1A的概括性描述了烟道气处理系统15的图,该烟道气处理系统15用于从在例如发电站的蒸汽发生器系统中所使用的锅炉系统26的燃烧室排出的烟道气流FG中去除多种污染物。该系统包括CO2去除系统70,其设计用来在将清洁烟道气排放到排气烟囱90之前(或者是附加的处理),从烟道气流FG中去除CO2。它也用来输出从烟道气流FG中去除的CO2。CO2去除系统70的细节概括地描述在图1B中。
参考图1B,CO2去除系统70包括用于从烟道气流FG中捕获/去除CO2的捕获系统72,和用于使用来从烟道气流FG中去除CO2的离子溶液再生的再生系统74。捕获系统72的细节概括地描述在图1C中。
参考图1C,概括描述了CO2捕获系统70(图1A)的CO2捕获系统72。该系统中,捕获系统72是基于冷冻氨的CO2捕获系统。在基于冷冻氨的去除CO2的系统/方法中提供吸收容器,在其中使吸收剂的离子溶液(离子溶液)与含CO2的烟道气流(FG)接触。离子溶液一般为含水的,可以由例如水和铵离子、碳酸氢根离子、碳酸根离子和/或氨基甲酸根离子组成。已知的CAP去除CO2系统的一个例子详细描述在图1C中。
参考图1C,吸收容器170用来接收来源于例如矿物燃料燃烧锅炉26(见图1A)的燃烧室的烟道气流(FG)。它也设计用于接收来自再生系统74(见图1B)的贫离子溶液供料。贫离子溶液通过液体分布系统122引入到容器170中,同时烟道气流FG也通过烟道气入口76被吸收容器170接收。
使离子溶液通过气液接触装置(在下文中,传质装置,MTD)111与烟道气流接触,该传质装置111用于传质并位于吸收容器170中,并在烟道气流从其入口76到容器出口77的流动路径中。气液接触装置111可以是例如一种或多种的已知结构化或随机组装的材料,或它们的组合。
离子溶液从喷头系统121和/或122喷出,向下喷射到传质装置111上面和/或内部。进料到喷头系统122的贫离子溶液和进料到喷头系统121的再循环离子溶液也可以组合并从一个喷头喷出。离子溶液多级流过(cascade through)传质装置111,与上升(与离子溶液方向相反)并穿过传质装置111的烟道气流FG接触。
一旦与烟道气流接触,离子溶液其从烟道气流中吸收CO2的作用,这使得离子溶液“富含”CO2(富溶液)。富离子溶液继续向下流动通过传质装置然后被收集于吸收容器170的底部78中。富离子溶液然后通过再生系统74(见图1B)再生,从而释放由离子溶液从烟道气流中吸收的CO2。从离子溶液中释放的CO2可以随后被输出至储存或其它预定的用会途/目的之用。一旦CO2从离子溶液中释放,离子溶液即称为“贫”。贫离子溶液随后准备再次从烟道气流中吸收CO2,可以引回到液体分布系统122藉此重新进入吸收容器170。
离子溶液通过喷头系统122喷入吸收容器170中之后,向下落到传质装置111上并通过它,在此处与烟道气流FG接触。一旦与烟道气流接触,离子溶液与烟道气流中可能含有的CO2反应。该反应是放热反应,从而在吸收容器170中产生热量。该热量可以导致离子溶液中包含的部分氨变为气体。气态氨然后,不随液体离子溶液一起向下移动,而是随后与烟道气流一起并作为烟道气流的一部分向上移动通过吸收容器170,最后通过吸收容器170的出口77逃逸。来自系统的氨的损耗(逃脱氨)减少了离子溶液中氨的摩尔浓度。由于氨的摩尔浓度降低,R值(NH3与CO2的摩尔比)也同样降低。
当烟道气流与离子溶液接触时,烟道气流中包含的二氧化碳与水(H2O)和氢氧离子(OH-)反应生成碳酸氢根离子。这种“捕获反应”(下面示出的反应1到反应9)大体描述如下:
(反应1)CO2(气)------→CO2(水溶液)
(反应2)CO2(水溶液)+2H2O------→HCO3 -(水溶液)+H3O+
(反应3)CO2(水溶液)+OH------→HCO3 -(水溶液)
NH3和它的离子以及CO2的反应发生在液相中,下文将讨论该反应。然而,在低温(通常低于70-80F)和高离子强度(通常为2-12M铵离子)下,反应(2)和反应(3)生成的碳酸氢根将与铵离子反应,当NH3/CO2之比小于2时根据下式,以碳酸氢铵而沉淀:
(反应4)HCO3 -(水溶液)+NH4 +(水溶液)------→NH4HCO3(固)
反应2是慢反应,而反应3是较快反应。在高pH水平例如pH高于10时,离子溶液中的OH-浓度高,因而通过反应(3)捕获了大部分CO2,能达到高的CO2捕获效率。在较低pH时,氢氧离子(OH-)浓度低,CO2捕获效率也低,主要基于反应(2)。
在基于冷冻氨的CO2捕获系统/方法中,通过使烟道气流与氨水溶液接触,让烟道气流中的CO2直接与氨水反应,来捕获烟道气流中的CO2。在低R(通常小于约2)和通常小于10的pH时,CO2与离子溶液中的氨的直接反应是捕获CO2的主导机制。CO2次序捕获中的第一步是反应(1)的CO2从气相到液相的传质。在液相中,CO2水溶液和氨水发生的反应顺序为:
(反应5)CO2(水溶液)+NH3(水溶液)------→CO2*NH3(水溶液)
(反应6)CO2*NH3(水溶液)+H2O------→NH2CO2 -(水溶液)+H3O+
(反应7)NH2CO2 -(水溶液)+H2O------→NH4 +(水溶液)+CO3 =(水溶液)
(反应8)CO3 =(水溶液)+NH4 +(水溶液)------→HCO3 -(水溶液)+NH3(水溶液)
(反应9)CO3 =(水溶液)+H3O+------→HCO3 -(水溶液)+H2O
如上面描述的,反应(8)和反应(9)生成的碳酸氢根可以基于反应(4)与铵离子反应,以作为固体碳酸氢铵沉淀,同时反应(8)中生成的氨可以基于反应(5)与另外的CO2反应。
连锁反应(5)到(9)的序列是比较慢,因而需要巨大且昂贵的CO2捕获装置。CO2的慢速吸收是由于:1)捕获反应序列(反应1到反应9)中的一个或多个低速反应;2)中间产物例如CO2*NH3和NH2CO2 -的累积在离子溶液中。中间产物的累积减慢了CO2捕获过程,并导致发电设备中的较低CO2捕获效率。因此,工业中仍存在对加速CO2捕获反应速率的至今尚未解决的需求,这显著地减少CO2捕获设备和辅助系统的尺寸和成本。
进一步地,本发明的特征通过说明书和权利要求将是显而易见的。
附图说明
参考附图可以更好地理解本发明的很多方面。图中的组件不需按比例绘制,重点而是放在清楚地说明本发明的原理上。此外,在图中,在全部多个视图中相同的参照数字来表示相应的组件。现在参考附图更详述本发明,附图中:
图1A是概括描述了包含CO2去除系统70的烟道气处理系统15的示意图。
图1B是概括描述了包含捕获系统72和再生系统74的CO2去除系统70的进一步细节的示意图。
图1C是概括描述捕获系统72的细节的示意图。
图2是说明其中离子溶液用于捕获CO2的捕获效率的曲线图(在有或没有助催化剂情况下)。
图3是概括描述捕获系统72的实施方案的示意图,其包括使离子溶液+助催化剂与烟道气流接触的吸收系统。
讨论
本发明涉及一种基于冷冻氨的CO2的捕获系统和方法。更具体地,本发明涉及基于冷冻氨的CO2的捕获系统和方法,其中使用助催化剂以帮助加速某些捕获反应,该反应与基于冷冻氨的离子溶液与含CO2的气流的接触基本上同步和/或由作为其结果而发生。
提出了一种从气流中去除CO2的系统和方法,其中提供基于冷冻氨的离子溶液,该离子溶液包含助催化剂以帮助加速某些在CO2和铵离子溶液之间发生的反应,所述反应基本上与基于冷冻氨的离子溶液和含CO2的气体流的接触同步发生和/或作为其结果而发生。在一个优选实施方案中,离子溶液与助催化剂混合。然后,通过例如CO2捕获吸收器/吸收容器,使离子溶液-助催化剂混合物与烟道气流接触。
助催化剂用作加速某些发生的“捕获反应”,也就是以下反应(反应5到反应9):
(反应5)CO2(水溶液)+NH3(水溶液)------→CO2*NH3(水溶液)
(反应6)CO2*NH3(水溶液)+H2O------→NH2CO2 -(水溶液)+H3O+
(反应7)NH2CO2 -(水溶液)+H2O------→NH4 +(水溶液)+CO3=(水溶液)
(反应8)CO3 =(水溶液)+NH4 +(水溶液)------→HCO3 -(水溶液)+NH3(水溶液)
(反应9)CO3 =(水溶液)+H3O+------→HCO3 -(水溶液)+H2O
通过加速捕获反应(5)到(9),提出的系统能在单位时间内从烟道气中捕获更多CO2,因而允许从烟道气中去除更多CO2。
在本发明的一个实施方案中,使用的助催化剂是胺。这种胺与离子溶液混合,并随后与含CO2的烟道气接触。用作助催化剂的可能的胺的一个例子包括但不限于哌嗪(PZ)。在另一个实施方案中,使用的助催化剂是酶或酶体系。这个实施方案中,酶或酶体系与离子溶液混合,并随后与含CO2的烟道气接触。可以用作助催化剂的酶或酶体系的一个例子包括但不限于Carbozyme渗透器,其可从Carbozyme,Inc of 1Deer Park Drive,Suite H-3,Monmouth Junction,NJ08852)得到。
哌嗪是一种C4N2H10环状化合物,在胺系统中已用作捕获CO2的助催化剂。实验发现,哌嗪是很好的与氨化溶液使用以增强CO2捕获和碳酸氢铵产量的助催化剂。在离子溶液中加入0.2-2.0摩尔PZ,优选0.4-1.0摩尔PZ,明显提高了CO2捕获效率。也提高碳酸氢铵固体颗粒从溶液中的沉淀。由于碳酸氢铵比溶液自身更富含CO2(固体颗粒中NH3/CO2之比为1.0),所以碳酸氢铵颗粒从溶液中沉淀提高了溶液的NH3/CO2之比和溶液的pH,产生了能捕获更多CO2的更贫的溶液。
通过PZ助催化剂在加速某些捕获反应中的作用,可以明显减少(差不多减少50-80%)CO2吸收容器和相关设备的物理尺寸。它还由于产生的吸收器的压降和液体循环率的降低,而减少了附加的能量消耗。简而言之,它能在低得多的成本下实施和操作有用的CO2捕获系统。
图2是表示在使用有和没有助催化剂(例如PZ)的离子溶液时,相对CO2捕获效率的曲线图。图2示显示了,与不用PZ相比,当使含有0.45MPZ的离子溶液通过11英尺的填装吸收器与烟道气流接触时,CO2捕获效率提高了。
图2中,在NH3/CO2摩尔比R=2.4时,具有0.45M PZ的CO2捕获效率是82%,而没有PZ时仅为51%。在R=2.0时,具有0.45M PZ的效率降至74%,没有PZ的降至仅36%。在R=1.8时,具有0.45M PZ的效率是66%,而没有PZ时仅为23%。在实验的操作条件下,在R=1.6时,具有0.45M PZ的效率仍高达52%,而不含PZ的效率小于10%。
PZ助催化剂在吸收和再生条件下都是稳定的,含PZ的再生溶液和新鲜的PZ溶液在多个CO2吸收循环中表现一样好。通过使用包含冷冻氨和助催化剂如哌嗪的吸收剂离子溶液,可以显著提高基于冷冻氨的CO2捕获系统的CO2捕获效率。哌嗪在低温吸收条件和高压高温再生条件下都是稳定的。再生后的含哌嗪的贫CO2溶液看起来与新鲜注入到含氨溶液中的哌嗪一样好。
图3概括描述了根据本发明的设计从烟道气流中捕获CO2的系统的一个实施方案。参考图3,吸收容器370设计以接收来源于例如矿物燃料燃烧锅炉26的燃烧室(见图1A)的烟道气流(FG)。它也被设计以接收来自再生系统74(见图1B)的贫离子溶液+助催化剂。贫离子溶液+助催化剂供料通过液体分布系统322送入容器370中,而烟道气流FG通过烟道气入口76也由吸收容器370接收。
离子溶液+助催化剂通过用于传质的气液接触装置(在下文中称为传质装置,MTD)311与烟道气流接触,该传质装置位于吸收容器370中,且位于烟道气流从入口76进入到容器出口77的流动路径上。气液接触装置311可以是例如一种或多种通常已知的结构化或随机填装的材料,或它们的组合。
离子溶液+助催化剂从喷头系统321和/或322喷出,向下降到传质装置311上面和/或内部。离子溶液多级流过(cascades through)传质装置311并与上升(与离子溶液+助催化剂方向相反)通过传质装置311的烟道气流FG接触。
一旦与烟道气流接触,离子溶液+助催化剂开始从烟道气流中吸收CO2,使得离子溶液+助催化剂“富含”CO2(富含的离子+助催化剂溶液)。富离子溶液+助催化剂继续向下通过传质装置,然后收集在吸收容器370的底部378中。
富离子溶液+助催化剂随后通过再生系统74(见图1B)再生,从而释放出由离子溶液从烟道气流中吸收的CO2。从离子溶液+助催化剂中释放出来的CO2然后可以被输出至储存或其它预定的用途/目的。一旦CO2从离子溶液+助催化剂中释放出来,该离子溶液+助催化剂被认为是“贫”的。贫离子溶液+助催化剂随后再次准备从烟道气流中吸收CO2,并可以送回液体分布系统122,藉此再次被引入吸收容器370中。
在离子溶液经喷头系统322喷入吸收容器370后,它多级流到传质装置311上并通过其,在那里与烟道气流FG接触。一旦与烟道气流接触,离子溶液+助催化剂与CO2反应从而从烟道气流中捕获和去除CO2。
需要强调的是,上面描述的本发明的实施方案,特别是任何“优选”的实施方案都只是可能的实施例,给出仅仅用来清楚理解发明的原理。对上面描述的本发明的实施方案可以进行很多变化和修改,而基本不脱离本发明的精神和原理。所有这些变化和修改在这里旨在被包括在本发明公开的范围之内,受到随后的权利要求书的保护。
Claims (9)
1.一种从烟道气中吸收CO2的方法,其包括以下步骤:
使助催化剂与吸收剂离子溶液(离子溶液)相组合;
使组合后的助催化剂和离子溶液与含CO2的烟道气流接触;以及
使组合后的助催化剂和离子溶液再生,以释放从烟道气中吸收的CO2。
2.权利要求1所述的方法,其中助催化剂包含胺。
3.权利要求1所述的方法,其中助催化剂包含酶体系。
4.权利要求2所述的方法,其中胺包含哌嗪。
5.权利要求3所述的方法,其中酶体系包含carbozyme渗透器。
6.一种从烟道气中吸收CO2的系统,包括:
设计用于接收烟道气流的吸收容器;
进一步设计用于接收吸收剂溶液供给的吸收剂容器;
吸收剂溶液包含与助催化剂混合的离子溶液;以及
该吸收容器包含设计用于使烟道气流与吸收剂溶液接触的气液传质装置(MTD)。
7.权利要求6所述的系统,其中吸收剂溶液包含冷冻氨和助催化剂。
8.权利要求7所述的系统,其中助催化剂包含哌嗪。
9.权利要求7所述的系统,其中助催化剂包含酶体系。
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- 2008-11-24 RU RU2010127268/04A patent/RU2481882C2/ru not_active IP Right Cessation
- 2008-11-24 EP EP08856753A patent/EP2227311A1/en not_active Withdrawn
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MX2010005801A (es) | 2010-08-02 |
EP2227311A1 (en) | 2010-09-15 |
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US8168149B2 (en) | 2012-05-01 |
AU2008331587A1 (en) | 2009-06-11 |
RU2481882C2 (ru) | 2013-05-20 |
JP2011506061A (ja) | 2011-03-03 |
US7862788B2 (en) | 2011-01-04 |
CA2798618A1 (en) | 2009-06-11 |
KR20100116582A (ko) | 2010-11-01 |
US20090148930A1 (en) | 2009-06-11 |
BRPI0820016A2 (pt) | 2015-05-19 |
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CA2707675A1 (en) | 2009-06-11 |
US20110070136A1 (en) | 2011-03-24 |
WO2009073422A1 (en) | 2009-06-11 |
CA2798618C (en) | 2013-12-31 |
WO2009073422A8 (en) | 2010-09-30 |
CA2707675C (en) | 2013-02-19 |
CN102083513B (zh) | 2013-09-18 |
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