CN103201015A - 用于从烟道气中捕捉co2的溶剂和方法 - Google Patents
用于从烟道气中捕捉co2的溶剂和方法 Download PDFInfo
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Abstract
本公开描述有效使用例如酶的催化剂,以对溶剂提供适当的实际循环容量,除非被它的吸收并且维持从烟道气中捕捉高浓度的CO2的能力所限制。本发明可应用于非促进以及促进溶剂并且应用于具有大范围反应焓的溶剂。
Description
本发明专利主张对在2010年9月15日申请的共同未决的美国临时申请第61/388,046号的优先权。
技术领域
本公开涉及用于从烟道气中捕捉(capture)二氧化碳(CO2)的催化增强溶剂的使用,从而避免需求促进剂或较高反应焓的溶剂。
背景技术
对于烟道气应用,工艺条件(烟道气的稀释CO2浓度、低分压力,低热容量)使得吸收工艺在对应放热反应期间被低吸收速率或被吸收器中温度的过度增长所限制。
在过去,这两个问题已经通过使用具有较高吸收焓的溶剂而解决。较高吸收焓与溶剂的较强碱性属性(较高的pKa)大致相关,并且因此与增长的反应速率以及溶剂中较高的CO2溶解性大致相关。特别地,使用胺基溶剂从烟道气中捕捉CO2中的某些主要工作推荐较高反应焓的溶剂用于烟道气应用[Rochelle]。
令人遗憾的是,较高反应焓的溶剂存在缺点,即它们参与溶剂的再生所需的能量的增加。吸收器中的CO2溶剂的改良亲合性在其开始在再生器中逆转反应时成为缺点。因此,存在需要处理的权衡(trade-off)。
发明内容
本发明涉及有效使用例如酶的催化剂,以减少与如上所述的权衡相关的约束,从而对溶剂提供适当的实际循环(cyclic)容量,除非被它的吸收并且维持从烟道气中捕捉高浓度的CO2的能力所限制。本发明可应用于非促进性(non-promoted)以及促进性溶剂并且应用于具有大范围反应焓的溶剂。
附图说明
图1是用于从气流中移除CO2的常规系统的示意图。
图2是作为不同胺的酸解离常数(pKa)的函数的(基于热力学CO2负荷容量(loading capacity/ 吸附容量))理论循环容量的图表。
具体实施方式
图1示出用于从气流中移除CO2的常规系统。系统包括吸收器柱(column)(吸收器)111,其中,包含CO2的气流(例如烟道气流)112例如以逆流模式与诸如胺基溶剂的溶剂溶液110接触。在吸收器中,来自气流的CO2被吸收在溶剂中。富CO2的已用溶剂经由路线101离开吸收器。富CO2溶剂经由热交换器109和路线102传递至再生器103,其中,已用溶剂通过破坏CO2与溶液之间的化学键而除去CO2。再生溶剂经由路线104离开再生器底部。移除的CO2和水蒸气在再生器的顶部处经由路线105离开工艺。另外,冷凝器可布置在再生器的顶部处以防止水蒸气离开工艺。
再生溶剂经由路线104传递至重沸器106。在位于再生器的底部处的重沸器中,再生溶剂被煮沸以产生蒸气107,其被返回至再生器以驱使从溶剂中分离CO2。另外,重沸可提供用于从再生溶剂中进一步移除CO2。
在重沸后,重沸且因而加热的溶剂经由路线108传递至热交换器109用于与来自吸收器的已用溶剂热交换。热交换容许溶液之间的传热,从而产生冷却的重沸溶剂和加热的已用溶剂。重沸且热交换的溶剂其后传递至吸收器中的下一轮吸收。在被供给至吸收器之前,溶剂110可被冷却至适于吸收的温度。因此,冷却器可布置在吸收器溶剂入口(未图示)附近。
常规胺基溶剂的示例包括例如胺化合物,诸如单乙醇胺(MEA)、二乙醇胺(DEA)、甲基二乙醇胺(MDEA)、二异丙基胺(DIPA)和氨基乙氧基乙醇(二甘醇胺)(DGA)。工业设备中的最常用胺化合物为链烷醇胺MEA、DEA、MDEA和常规胺与促进剂(例如哌嗪(piperazine))和/或抑制剂的某些混合物。
用于烟道气应用的典型胺基溶剂在大约100-140华氏度的温度下吸收CO2。低于该下限温度,吸收的动力被限制或减缓,高于该上限温度,溶剂中CO2的溶解性快速变小。由于吸收反应的放热性质,故吸收器内的溶剂的温度可高于它的入口或出口温度。这可导致内部热力学收缩(thermodynamic pinch)和用于传质(mass transfer)的吸收器柱的低利用率。
本发明针对如下溶剂,其具有(基于热力学CO2负荷容量)相对高的理论循环容量,例如大于大约1摩尔/升的循环容量,但是具有在实际工艺条件(低吸收速率和/或由于吸收器中的放热反应的温变溶解性)下吸收CO2的有限能力,从而不实现理论循环容量的显著百分比。例如,图2是作为不同胺的酸解离常数(pKa)的函数的理论循环容量的图表。如图2所示,诸如例如DMEA(二甲基乙醇胺)、DEEA(二乙基乙醇胺)和DMgly(二甲基甘氨酸)的其他叔胺可具有高于MDEA的循环容量。我们已经观察到这些胺典型地具有在大约9到大约10.5的范围中的pKa(40℃)。在曲线顶部处的胺具有大于MDEA的容量,但是先前被认为太慢以不能在适度大小的吸收器中反应。
通过使用增强较低温度下CO2吸收的动力的催化剂,可优化吸收器中的工艺条件以将溶剂的实际循环容量增加至理论循环容量(如由热力学所限定的)的较高百分比。此种催化剂可包括例如生物催化剂,诸如碳酸酐酶或它的相似物。不存在温度应该为多低、催化剂应在某温度下增强动力的限制,然而,从实用观点看,可推荐如下温度范围。催化剂应当容许在80-140华氏度的范围中的温度下实现与非催化溶剂相比增加的CO2负荷。特别地,对于任何溶剂,容许在更低温度下而实现相同或更高吸收速率的催化剂是有益的。
使用催化增强溶剂,可通过以下方式完成用于更高循环容量的工艺的优化:
●降低进入吸收器的溶剂的入口温度。因而整个柱更冷,从而提高CO2的溶解性而不损害吸收速率。这导致与非催化溶剂相比增长的实际富负荷而非固定贫负荷;
●通过使用中间冷却(例如,吸收器塔内的冷却盘管或其他热交换器)和/或中间冷却-再循环(例如,从吸收器塔中抽出溶剂的部分,冷却该部分,并且将它重新注入回吸收器柱中)降低吸收器内的溶剂温度。柱的一部分因而更冷,从而提高CO2的溶解性,而不损害吸收速率。这导致与非催化溶剂相比增长的实际富负荷而非固定贫负荷;
●降低液-气流动速率比。这可通过容许与放热反应相关的温度凸升(bulge)在吸收器的顶部处而促进吸收器柱的底部中的较低温度。柱的一部分因而更冷,从而增加CO2的溶解性而不损害吸收速率。这导致与非催化溶剂相比增长的实际富负荷而非固定贫负荷。
示例
在该示例中选择催化增强MDEA并且将其与Pz扮演促进剂角色的MDEA-Pz相比较。这仅用于说明,本发明可适用于MDEA、MDEA-Pz,并且通常可适用于呈现用于从烟道气中分离特定程度CO2的足够高的理论循环容量的任何溶剂。
下面,在特定工艺温度和特定烟道气成分下比较MDEA和MDEA-Pz的理论循环容量:
●15kPa的CO2分压(PCO2)入口烟道气
MDEA的溶剂理论循环容量为:
●95华氏度下为0.38
●105华氏度下为0.32
●115华氏度下为0.27
●125华氏度下为0.22
MDEA-Pz的溶剂理论循环容量为:
●95华氏度下为0.47
●105华氏度下为0.44
●115华氏度下为0.39
●125华氏度下为0.36
对于本申请,建议从烟道气中移除90%。选定液气比为3.36kg/hr/kg/hr,对于MDEA-Pz,最小实际循环容量为~0.30mol CO2/mol胺,对于MDEA,最小实际循环容量为~0.32mol CO2/mol胺。
因此,在所有温度(95-125华氏度)下,MDEA-Pz理论上可实现分离,而MDEA仅可在95华氏度下实现分离。用于MDEA溶剂的液气比可增加以使用小于0.32mol/mol的循环容量实现捕捉速率,但是这需求较高液气比和对应的增长能量损害。在表格1和表格2中报告该对应的增长能量损害。
表格1:与使用MDEA-Pz从包含15kPa CO2的烟道气中捕捉90%CO2相关的重沸器效率
表格2:与使用MDEA从包含15kPa CO2的烟道气中捕捉90%CO2相关的重沸器效率
从这两个表格可以看出,与具有较高反应焓的促进溶剂相比,对MDEA提供等于理论循环容量的循环容量的催化剂容许减少的能量损害。在该特定情况下,与MDEA-Pz溶剂的~70-80kJ/mol CO2相比,预计催化MDEA具有42kJ/mol CO2的反应焓。还可注意到充分增强动力以在低温下(在本情况下为95华氏度)实现理论循环容量的催化剂在与促进溶剂相同的溶剂循环速率(液气比)下提供改良能量数量。然而,若催化剂工作的温度提高,则只能与促进催化剂相比以更高液气比和能量节约方面的对应减少的成本来实现分离(在本情况下,在95华氏度下,在能量需求方面减少15%,与此相对,在125华氏度下,在能量需求方面仅减少6%)。
在实际应用中,不预期可实现理论循环容量。由于容积限制和接触时间限制,实际循环容量将仅为理论循环容量的百分比。在表格3和4中,示范了催化剂如何通过在吸收器底部柱处影响能够实现的对热力学平衡的接近而能够改良溶剂的能量性能。工艺条件保持与先前列出的工艺条件相同。
表格3:作为在吸收器出口处的能够实现的CO2负荷的函数的MDEA-Pz的能量需求
*平衡接近值(Approach to equlibrium)
表格4:作为在吸收器出口处的能够实现的CO2负荷的函数的催化MDEA的能量需求
*平衡接近值
对于代表性的70-80%的平衡近似值,与Pz促进MDEA相比,当使用催化增强MDEA时,95华氏度下的能量需求方面的减少为18%和21%之间。
在高于95华氏度的温度下(在此未示出),可预期相同趋势,然而,由于需要与溶剂的更低循环容量相关的更高溶剂循环速率,故预期能量降低方面的益处更少。
在上面的示例中,示范了诸如MDEA的催化增强溶剂可优于化学促进溶剂(诸如MDEA-Pz)地工作。若催化增强发生在充分低的温度下,则能够实现20%或更多的能量损害减少。在较高温度下也可看到益处,但是由于溶剂循环速率需要增加以实现特定CO2分离度(例如90%),故预期能量减少。本发明可应用于任何促进胺基溶剂。本发明最适合于具有较低反应焓的溶剂。
虽然本发明已参考各种示范实施例而说明,但是本领域技术人员将理解,可进行各种变更并且等同物可被替换其中的元件,而不脱离本发明的范围。另外,可进行许多更改以使特定环境或材料适应本发明的教导,而不脱离本发明的实质范围。因此,意图为本发明不限于作为用于实现本发明而设想的最佳实施方式所公开的特定实施例,而是本发明将包括落入所附权利要求的范围内的所有实施例。
Claims (26)
1. 一种用于从烟道气流中捕捉CO2的溶剂溶液,所述溶剂溶液包括:
胺溶剂;和
催化剂,其在80-140华氏度范围中的温度下,与非催化溶剂相比,在所述胺溶剂中实现增长的CO2负荷。
2. 根据权利要求1所述的溶剂溶液,其特征在于,所述催化剂为生物催化剂。
3. 根据权利要求1所述的溶剂溶液,其特征在于,所述生物催化剂为碳酸酐酶或其类似物。
4. 根据权利要求1所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约1摩尔/升的理论循环容量。
5. 根据权利要求1所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约9并且小于或等于大约10.5的酸解离常数(pKa)。
6. 根据权利要求1所述的溶剂溶液,其特征在于,所述胺溶剂选自包括DMEA(二甲基乙醇胺)、DEEA(二乙基乙醇胺)和DMgly(二甲基甘氨酸)的组。
7. 一种降低用于使用胺溶剂从烟道气流中捕捉CO2的系统的能量需求的方法,所述方法包括:
将贫CO2溶剂溶液施加至吸收器柱中的富CO2烟道气流,以提供富CO2溶剂溶液和贫CO2烟道气流,所述溶剂溶液包括:
胺溶剂;和
催化剂,其在80-140华氏度范围中的温度下,与非催化溶剂相比,在所述胺溶剂中实现增长的CO2负荷;并且
降低提供至所述吸收器柱的所述贫CO2溶剂溶液的温度,从而提高所述吸收器柱内的CO2的溶解性。
8. 根据权利要求7所述的溶剂溶液,其特征在于,所述催化剂为生物催化剂。
9. 根据权利要求7所述的溶剂溶液,其特征在于,所述生物催化剂为碳酸酐酶或其类似物。
10. 根据权利要求7所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约1摩尔/升的理论循环容量。
11. 根据权利要求7所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约9并且小于或等于大约10.5的酸解离常数(pKa)。
12. 根据权利要求7所述的溶剂溶液,其特征在于,所述胺溶剂选自包括DMEA(二甲基乙醇胺)、DEEA(二乙基乙醇胺)和DMgly(二甲基甘氨酸)的组。
13. 一种降低用于使用胺溶剂从烟道气流中捕捉CO2的系统的能量需求的方法,所述方法包括:
将贫CO2溶剂溶液施加至吸收器柱中的富CO2烟道气流,以提供富CO2溶剂溶液和贫CO2烟道气流,所述溶剂溶液包括:
胺溶剂;和
催化剂,其在80-140华氏度范围中的温度下,与非催化溶剂相比,在所述胺溶剂中实现增长的CO2负荷;并且
降低所述吸收器柱内的所述溶剂溶液的温度,从而提高所述吸收器柱内的CO2的溶解性。
14. 根据权利要求13所述的方法,其特征在于,使用如下中的至少一种降低所述溶剂温度:所述溶剂溶液的再循环和中间冷却;所述溶剂溶液的再循环。
15. 根据权利要求13所述的溶剂溶液,其特征在于,所述催化剂为生物催化剂。
16. 根据权利要求13所述的溶剂溶液,其特征在于,所述生物催化剂为碳酸酐酶或其类似物。
17. 根据权利要求13所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约1摩尔/升的理论循环容量。
18. 根据权利要求13所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约9并且小于或等于大约10.5的酸解离常数(pKa)。
19. 根据权利要求13所述的溶剂溶液,其特征在于,所述胺溶剂选自包括DMEA(二甲基乙醇胺)、DEEA(二乙基乙醇胺)和DMgly(二甲基甘氨酸)的组。
20. 一种降低用于使用胺溶剂从烟道气流中捕捉CO2的系统的能量需求的方法,所述方法包括:
将贫CO2溶剂溶液施加至吸收器柱中的富CO2烟道气流,以提供富CO2溶剂溶液和贫CO2烟道气流,所述溶剂溶液包括:
胺溶剂;和
催化剂,其在80-140华氏度范围中的温度下,与非催化溶剂相比,在所述胺溶剂中实现增长的CO2负荷;并且
降低所述吸收器内的所述贫CO2溶剂和所述富CO2烟道气流的流动速率比,以通过容许与所述贫CO2溶剂与所述富CO2烟道气流之间的放热反应相关的温度凸升在所述吸收器的顶部区域处而促进所述吸收器柱的底部区域处的较低温度。
21. 根据权利要求20所述的方法,其特征在于,使用如下中的至少一种降低所述溶剂温度:所述溶剂溶液的再循环和中间冷却;所述溶剂溶液的再循环。
22. 根据权利要求20所述的溶剂溶液,其特征在于,所述催化剂为生物催化剂。
23. 根据权利要求20所述的溶剂溶液,其特征在于,所述生物催化剂为碳酸酐酶或其类似物。
24. 根据权利要求20所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约1摩尔/升的理论循环容量。
25. 根据权利要求20所述的溶剂溶液,其特征在于,所述胺溶剂具有大于或等于大约9并且小于或等于大约10.5的酸解离常数(pKa)。
26. 根据权利要求20所述的溶剂溶液,其特征在于,所述胺溶剂选自包括DMEA(二甲基乙醇胺)、DEEA(二乙基乙醇胺)和DMgly(二甲基甘氨酸)的组。
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US20140106440A1 (en) * | 2011-06-10 | 2014-04-17 | Co2 Solutions Inc. | Enhanced enzymatic co2 capture techniques according to solution pka, temperature and/or enzyme character |
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US9409120B2 (en) | 2014-01-07 | 2016-08-09 | The University Of Kentucky Research Foundation | Hybrid process using a membrane to enrich flue gas CO2 with a solvent-based post-combustion CO2 capture system |
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