CN113731489A - 一种用于富二氧化碳胺溶液再生的离子液体催化剂 - Google Patents
一种用于富二氧化碳胺溶液再生的离子液体催化剂 Download PDFInfo
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- B01J31/0278—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides comprising ionic liquids, as components in catalyst systems or catalysts per se, the ionic liquid compounds being used in the molten state at the respective reaction temperature containing nitrogen as cationic centre
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Abstract
本发明公开了一种用于富二氧化碳胺溶液再生的离子液体催化剂。在富胺溶液反应过程中,酸性离子液体催化剂加入到反应体系中,且所述富胺溶液解吸反应中的离子液体催化剂的阳离子为咪唑阳离子,阴离子为酸性阴离子。本发明方案在氨基甲酸酯解吸二氧化碳反应过程中,添加均相离子液体催化剂,不仅实现了二氧化碳的快速解吸,还可以有效降低解吸反应所需温度;同时该方法操作简单,能耗小,成本低,具有很强的工业实用性。
Description
技术领域
本发明涉及一种用于富二氧化碳胺溶液再生的离子液体催化剂,属于资源与环境技术领域。
背景技术
随着大量化石燃料的燃烧和人类活动的增加,导致温室效应和全球变暖。目前,我国还是以燃煤发电和火力发电为主,燃煤机组是CO2的集中排放源,如果不采取有效措施加以控制,其持续排放的CO2将给我国带来能源及气候变化等方面的压力。碳捕集与封存(CCS)技术成为减少CO2排放的潜在选择,可实现CO2的零排放或几乎不排放。其中,单乙醇胺(MEA)溶液具有CO2反应速率快,价格低廉等优点,是目前应用最为广泛、技术最为成熟的捕获剂之一。但其再生能耗高,解吸操作费用约占总操作费用的70%-80%。胺溶剂再生能耗居高不下是目前胺法CO2捕获技术所面临的最大问题,它极大地阻碍了该技术的工业化应用。因此,促进富胺溶剂的再生过程,降低其再生能耗具有重要的研究意义。
为了降低胺溶剂捕集CO2工艺的再生能耗,研究学者提出添加固体酸催化剂来促进胺溶剂的再生过程,降低其再生能耗。Shi等人研究了催化剂HZSM-5 和γ-Al2O3对MEA及MEA-DEAB(4-(二乙胺)-2-丁醇))体系的CO2解吸性能的影响,结果表明,固体酸催化剂可以降低富MEA的再生能耗,而催化剂和混合胺的耦合则能够进一步的降低CO2的解吸能耗(Shiet al.International Journal of Greenhouse Gas Control.2014,26:39–50)。Prasongthum等人研究了超强固体酸催化剂Ce(SO4)2/ZrO2的催化胺溶液再生性能,结果表明因其突出的 Bronsted酸性位点(B酸)而表现出较好的催化解吸性能(Prasongthum etal. Energy Fuels.2019,33:1334-1343)。Wang等人研究了SiO2、Al2O3和TiO2三种纳米颗粒对MEA溶液再生过程的影响,结果显示相对空白解吸,TiO2的添加可以节省42%的解吸时间(Wang et al.Ind.Eng.Chem.Res.2016,55:7830-7838)。
离子液体具有明显的“绿色”环保性质,在催化反应过程中,可以替代有毒、污染严重的传统非环保型催化剂,实现良好的社会和经济效应。同时具有液体酸的高密度反应活性和固体酸的不挥发性,以及均相催化效率高的优点,在催化领域备受关注。因此,利用离子液体的酸性及表面活性促进富胺溶液低能耗解吸,代替常规酸催化剂,对CCUS技术而言具有重大的应用潜力和工业需求。
发明内容
本发明解决的技术问题是,通过添加酸性离子液体催化剂,进一步提高胺溶液解吸速率,降低富二氧化碳胺溶液再生能耗,从而降低有机胺法捕获CO2运行成本,实现能源的多效利用,达到节能减排的目的。
本发明的技术方案是,提供一种用于富二氧化碳胺溶液再生的离子液体催化剂。该方法可以提高二氧化碳解吸速率,降低胺溶液再生的能耗。
本发明提供的一种用于富二氧化碳胺溶液再生的离子液体催化剂,应用于有机胺法捕获二氧化碳工艺过程中,其特征在于,所述胺溶液为单乙醇胺。
优选地,单乙醇胺浓度为5M。
优选地,富二氧化碳胺负载量为0.45~0.55mol CO2/mol胺。
优选地,反应温度为90℃。
优选地,离子液体催化剂加入含量为富胺溶液的0.5~5wt.%。
优选地,所述的离子液体为1-丁基-3-甲基咪唑硫酸氢盐([BMIM][HSO4])、 1-丁基-3-甲基咪唑六氟磷酸盐([BMIM][PF6])、1-丁基-3-甲基咪唑溴酸盐([BMIM]Br)、1-丁基-3-甲基咪唑氯盐([BMIM]Cl)、1-丁基-3-甲基咪唑四氟硼酸盐([BMIM][BF4])。
本发明提供的离子液体为催化剂的富二氧化碳胺溶液再生反应方法,用于传统有机胺法捕获CO2工艺中富胺再生过程,可极大的降低再生能耗。其主要原因在于,富CO2胺溶液解吸过程需要酸性位点,使得离子液体催化剂在催化富胺溶液再生过程中具有良好的催化性能。
与现有技术相比,本项目具有如下技术优势和有益效果:
(1)催化剂原料廉价易得。
(2)催化解吸性能优越。
(3)反应条件温和,操作简便。
(4)离子液体催化剂具有“绿色”环保性质,可以替代有毒、污染严重的传统催化剂,具有良好的社会和经济效应。
附图说明
图1表示富CO2胺溶液间歇式解吸装置图。
图2表示CO2解吸过程的相对能耗图。
具体实施方式
为了更好的阐述本发明为达到预定的发明目的所采取的技术手段可行,将结合附图,对本发明提出的离子液体为催化剂的富二氧化碳胺溶液再生反应方法及具体实施方式进行详细说明。
实施例1
富CO2胺溶液再生的实验室规模间歇式解吸装置如图1所示,容积为1L 的圆底烧瓶作为CO2解吸反应的反应器。采用磁力搅拌使得气液两相拥有充分的接触面积,同时保证胺溶液的浓度及温度能够处于较为均匀的状态。圆底烧瓶的两个接口分别连接温度探针和冷凝器,冷凝器的使用是为了防止胺溶液的挥发,确保胺溶液的浓度能够维持在一定范围内。温度探针时刻监测再生胺溶液的温度,控温精度为±0.1℃的加热套用来提供解吸反应所需要的热量。通过质量流量计控制出口混合气体(N2和脱除CO2气体)的流量。混合气体中N2和CO2的浓度由CO2红外分析仪实时监测。在实验过程中,将加热套和电能表进行串联,利用电能表来记录消耗的电量以此来计算CO2解吸过程的相对解吸能耗。解吸所用的胺溶液浓度为5M,富液负载约为0.51mol CO2/mol amine,搅拌速率设为1200rpm,所用离子液体催化剂为1-丁基-3-甲基咪唑硫酸氢盐 ([BMIM][HSO4])。具体操作过程如下,将500mL的富MEA溶液和4.53g(重量比约为0.91wt.%)的催化剂一同加入到圆底烧瓶中,解吸温度设为25-90℃,每次解吸持续1h,分析前20min的解吸过程。
实施例2
同实施例1,其区别在于所用离子液体催化剂为1-丁基-3-甲基咪唑六氟磷酸盐([BMIM][PF6])。
实施例3
同实施例1,其区别在于所用离子液体催化剂为1-丁基-3-甲基咪唑溴酸盐([BMIM]Br)。
实施例4
同实施例1,其区别在于所用离子液体催化剂为1-丁基-3-甲基咪唑氯盐 ([BMIM]Cl)。
实施例5
同实施例1,其区别在于所用离子液体催化剂为1-丁基-3-甲基咪唑四氟硼酸盐([BMIM][BF4])。
表1实施例中的催化剂解吸能耗比较
催化剂 | 能耗比值(%) | 能耗降低(%) |
空白 | 100 | - |
实施例1:[BMIM][HSO<sub>4</sub>] | 95.47 | 4.53 |
实施例2:[BMIM][PF<sub>6</sub>] | 87.44 | 12.56 |
实施例3:[BMIM]Br | 87.50 | 12.50 |
实施例4:[BMIM]Cl | 94.36 | 5.64 |
实施例5:[BMIM][BF<sub>4</sub>] | 88.16 | 11.84 |
由上表可知,相对于空白MEA,加入催化剂均显著降低了MEA解吸能耗。
Claims (6)
1.一种用于富二氧化碳胺溶液再生的离子液体催化剂,该富胺溶液再生反应应用于有机胺法捕获二氧化碳工艺过程中,其特征在于,所述胺溶液为单乙醇胺(MEA)。
2.根据权利要求1所述的方法,其特征在于,单乙醇胺浓度为2~6M,优选5M。
3.根据权利要求1所述的方法,其特征在于,富二氧化碳胺负载量为0.45~0.55molCO2/mol胺。
4.根据权利要求1所述的方法,其特征在于,反应温度在70~130℃之间,优选90℃。
5.根据权利要求1所述的方法,其特征在于,离子液体催化剂加入含量为富胺溶液的0.5~5wt.%。
6.根据权利要求1所述的方法,其特征在于:所述的离子液体为1-丁基-3-甲基咪唑硫酸氢盐([BMIM][HSO4])、1-丁基-3-甲基咪唑六氟磷酸盐([BMIM][PF6])、1-丁基-3-甲基咪唑溴酸盐([BMIM]Br)、1-丁基-3-甲基咪唑氯盐([BMIM]Cl)、1-丁基-3-甲基咪唑四氟硼酸盐([BMIM][BF4])。
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