CN115069068A - 一种水滑石类催化剂催化叔胺溶剂快速低能耗捕获co2的方法 - Google Patents
一种水滑石类催化剂催化叔胺溶剂快速低能耗捕获co2的方法 Download PDFInfo
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Abstract
本发明公开了一种快速、低能耗捕获CO2的方法，具体是采用水滑石催化剂催化叔胺溶剂来捕获CO2。相较于传统的叔胺溶剂CO2吸收工艺，本发明提供的方法可极大地提升CO2吸收速率、进而实现低能耗CO2捕获过程。与现有技术相比催化剂廉价易得；催化叔胺溶剂CO2吸收性能优越，且循环稳定性优异；反应条件温和，操作简便；水滑石类催化剂具有大表面积、多孔性、高的水热稳定性、良好的表明碱性位点等优点，可以替代价格昂贵且易失活的碳酸酐酶等催化剂，具有良好的社会和经济效益。
Description
技术领域
本发明属于气体分离技术领域，具体涉及一种水滑石类催化剂催化叔胺溶剂快速低能耗捕获CO2的方法。
背景技术
化石能源的大量燃烧向大气中排放过量的二氧化碳(CO2)，这是造成温室效应的重要原因。目前，有机胺溶液化学吸收法具备吸收容量大、设备投入小、价格低廉及成熟度高等优点，被认为是短期内最有可能应用于燃煤电厂的CO2捕集技术。然而，现有的有机胺吸收工艺存在能耗高、溶剂降解及腐蚀设备等不足。其中，伯胺吸收剂再生能耗占总捕集成本的60％，因此，降低CO2捕集成本以促进其进一步工业化应用的关键在于降低有机胺溶剂的再生能耗。
根据分子中与氮原子相连的氢原子数目，有机胺可分为伯胺、仲胺和叔胺。典型的伯胺如单乙醇胺(MEA)，CO2与MEA进行化学反应，形成氨基甲酸离子。伯胺溶剂CO2吸收速率快，但因氨基甲酸酯难以断裂，导致其解吸能耗过大，是目前这两类吸收剂在工业上广泛应用的瓶颈问题。此外，伯胺溶剂还存在吸收容量低及溶剂易降解等不足。仲胺溶剂虽然具有不易降解及沸点较高可在较高温度下吸收CO2等优点，但存在吸收速率低、脱除效率低及价格昂贵等不足。另一方面，叔胺溶剂如，N-甲基二乙醇胺(MDEA)，因不直接与CO2进行反应，而是通过碱催化机理，促进CO2水合反应，最终生成碳酸、碳酸氢根和质子化胺。因碳酸根及碳酸氢根不稳定，容易分解生成CO2，因此叔胺溶剂再生能耗低，且叔胺溶剂还具有CO2吸收容量大、抗降解性能优异等优势。因此，叔胺溶剂是一类十分有潜力的低能耗CO2吸收剂。然而，由于叔胺溶剂吸收CO2的速率过慢，限制了其大规模实际应用。
针对叔胺溶剂CO2吸收速率过低的问题，研究者提出碳酸酐酶(CA)催化剂能够有效加快CO2水合速率，降低CO2吸收焓。CA催化CO2水合生成HCO3-的能力已被大量研究所证明，CA是已知的催化CO2水合速率最快的酶(Wu et al.,Chinese J.Chem.Eng.,2020,28(11), 2817-2831.)。例如，Shen等人提出将CA酶嵌入到ZIF-L的纳米颗粒中，形成了一个新的 CA/ZIF-L-1复合材料，并用于CO2吸收过程，该复合材料对CO2的吸收显示了较好的催化活性(Shen et al.,Appl.Energy 2018,230,726-733)。Power等人开发了一种核壳磁性ZIF-8@Fe3O4-碳酸酐酶复合材料，以促进叔胺吸收CO2性能，研究了具有三种颗粒尺寸的CA@ZIF8@Fe3O4的催化性能。结果表明，CA@ZIF-8@Fe3O4的相对催化活性可高达95.2％(Power et al.,Environ.Sci.Technol.2016,50(5),2610-2618)。然而，CA自身的热稳定性低、循环性能差及价格昂贵等不足限制了其工业应用(Luis et al.,J.CO2 Util.,2021,47,101475；Rasouli et al.,Sep.Purif.Technol.2022,296,121299)。
因此，开发廉价、高效且稳定性优异的催化剂促进叔胺溶剂CO2吸收性能，获得高吸收速率、低能耗的CO2捕获方法，具有十分重要的理论意义和应用价值。
发明内容
针对现有技术的缺陷，本发明旨在提供一种快速、低能耗捕获CO2的方法，具体是采用水滑石催化剂催化叔胺溶剂来捕获CO2。相较于传统的叔胺溶剂CO2吸收工艺，本发明提供的方法可极大地提升CO2吸收速率、进而实现低能耗CO2捕获过程。其主要原因在于，基于碱催化机理，碱性水滑石类催化剂的加入，可提供CO2水合反应所需要的碱性位点，促进CO2水合反应的进行，促进叔胺溶剂CO2吸收速率。
本发明采用的CO2吸收体系包括催化剂和叔胺水溶液，把含有CO2的气体通入吸收体系，CO2首先被溶解，再被催化水合吸收，最终达到捕获CO2的目的。
本发明采用的催化剂可以选择镁铝水滑石(Mg/Al-LDH)及其对应的复合氧化物(Mg/Al-LDO)、钙铝类水滑石(Ca/Al-LDH)及其对应的复合氧化物(Ca/Al-LDO)的一种或者几种，但是优选使用Mg/Al-LDH。
本发明采用的催化剂用量范围为叔胺水溶液质量比的0-5wt％，优选使用1-2wt％，进一步优选使用1.25wt％。
本发明采用的反应温度为25-50℃。
本发明采用的叔胺溶剂可以是MDEA、二甲基氨基乙醇(DMEA)、4-二乙基-2-丁醇(DEAB)、1-二乙氨基-2-丙醇(1DEA2P)、1-(2-羟乙基)吡咯烷(1-(2-HE)PRLD)、1-(2- 羟乙基)哌啶(1-(2-HE)PP)、4-乙基-甲基-氨基-2-丁醇(EMAB)、三乙醇胺(TREA)、三乙基胺(TEA)、4-二乙胺基-2-丁醇(DEAB)、3-二甲胺基-1-丙醇(3DMA1P)、1-二甲胺基-2- 丙醇(1DMA2P)、N-甲基-4-哌啶(MPDL)、四甲基二乙胺(TMEDA)、四甲基二丙胺(TMPDA)、四甲基二丁胺(TMBDA)、4-氨基-1-甲基哌啶(4-A1MPD)、N,N-二乙基乙醇胺(DEEA)等的一种或者几种胺的混合溶剂，但是优选使用MDEA溶剂。
本发明采用的叔胺水溶液中包含的叔胺溶剂的质量比为10-40wt％。
本发明所述的包含CO2的气体是燃煤电厂排放的烟道气，CO2含量为10-20vol％，N2 含量为85-90vol％。
本技术主要有以下优势：
(1)催化剂廉价易得。
(2)催化叔胺溶剂CO2吸收性能优越，且循环稳定性优异。
(3)反应条件温和，操作简便。
(4)水滑石类催化剂具有大表面积、多孔性、高的水热稳定性、良好的表明碱性位点等优点，可以替代价格昂贵且易失活的碳酸酐酶等催化剂，具有良好的社会和经济效益。
附图说明
图1表示实施例中催化剂催化叔胺溶液CO2吸收速率图。
图2表示实施例中催化剂催化叔胺溶液CO2吸收量图。
图3表示实施例中催化剂的X射线衍射谱图。
图4表示实施例中催化剂的红外光谱谱图。
图5表示实施例中催化剂的氮气等温吸脱附曲线图。
图6表示实施例中叔胺溶液吸收CO2装置示意图。
具体实施方式
实施例1：Mg/Al-LDO、Ca/Al-LDO催化剂的制备及催化性能测试
(1)催化剂制备：将5g Mg/Al-LDH与Ca/Al-LDH催化剂置于坩埚并放入马沸炉中，在 500℃下焙烧3h，得到Mg/Al-LDO与Ca/Al-LDO催化剂。
(2)催化剂表征：对获得的催化剂进行，X射线衍射分析、红外光谱及N2吸脱附曲线等表征测试。
(3)催化性能测试：催化剂催化叔胺溶液CO2吸收实验装置如图4所示。实验步骤描述如下：称取一定量MDEA溶液于1L容量瓶中定容，并将溶液摇晃均匀，得到20％的MDEA 溶液。用量筒量取200ml 20％的MDEA溶液于三颈烧瓶内，再用电子天平称取2.5g Mg/Al-LDH于MDEA溶液。使用两个质量流量器，分别控制CO2和N2的流量为500mL/min，总流量为1000mL/min。把阀门打到双通道，将CO2和N2混合5min，再通入MDEA溶液中。连接三颈***玻璃管为砂芯玻璃管，可以使CO2以分散的小气泡形式进MDEA溶液，同时打开磁子搅拌，转速设为500rpm，使溶液和气体混合得更加均匀。通过MDEA溶液的混合气体，经过干燥管，去除夹带的水分，防止其对CO2含量的测量结果造成影响。干燥后的混合气体，进入CO2检测装置，记录CO2出口体积分数，吸收温度设为25℃，实验时长设为1h。
实施例2：
同实施例1中的催化性能测试，其区别在于叔胺溶液吸收CO2过程添加的催化剂为Mg/Al-LDH。
对比例：
同实施例1中的催化性能测试，其区别在于叔胺溶液吸收CO2过程未添加催化剂。
表1实施例和对照例的催化剂催化叔胺溶液吸收CO2瞬时提升速率及CO2瞬时提升量比较
| 吸收时间(s) | 催化剂 | 瞬时提升速率比值(％) |
| 空白吸收 | 0 | |
| 545/1055 | Mg/Al-LDH | 102.0/38.6 |
| 2145/2560 | Mg/Al-LDO | 17.7/7.7 |
| 3385/3585 | Ca/Al-LDO | 23.0/0.5 |
由表1，图1和图2可知，相对于空白MDEA溶液CO2吸收过程，加入碱性催化剂均显著地提升了MDEA溶液的CO2吸收速率和吸收量，其中Mg/Al-LDH催化剂的加入，可提升 CO2瞬时吸收速率102％。
Claims (6)
1.一种快速、低能耗捕获CO2的方法，把含有CO2的气体通入吸收体系，CO2首先被溶解，再被催化水合吸收，最终达到捕获CO2的目的。其特征在于，所述捕获方法包括催化剂和叔胺水溶液。所述的催化剂可以选择镁铝水滑石(Mg/Al-LDH)及其对应的复合氧化物(Mg/Al-LDO)、钙铝类水滑石(Ca/Al-LDH)及其对应的复合氧化物(Ca/Al-LDO)的一种或者几种，但是优选使用Mg/Al-LDH。
2.根据权利要求1所述的捕获方法，其特征在于，所述的催化剂用量为叔胺水溶液质量比的0-5wt％，优选使用1-2wt％，进一步优选使用1.25wt％。
3.根据权利要求1所述的捕获方法，其特征在于，所述吸收反应的温度为25-50℃。
4.根据权利要求1所述的捕获方法，其特征在于，所述的叔胺溶剂可以是MDEA、二甲基氨基乙醇(DMEA)、4-二乙基-2-丁醇(DEAB)、1-二乙氨基-2-丙醇(1DEA2P)、1-(2-羟乙基)吡咯烷(1-(2-HE)PRLD)、1-(2-羟乙基)哌啶(1-(2-HE)PP)、4-乙基-甲基-氨基-2-丁醇(EMAB)、三乙醇胺(TREA)、三乙基胺(TEA)、4-二乙胺基-2-丁醇(DEAB)、3-二甲胺基-1-丙醇(3DMA1P)、1-二甲胺基-2-丙醇(1DMA2P)、N-甲基-4-哌啶(MPDL)、四甲基二乙胺(TMEDA)、四甲基二丙胺(TMPDA)、四甲基二丁胺(TMBDA)、4-氨基-1-甲基哌啶(4-A1MPD)、N,N-二乙基乙醇胺(DEEA)等的一种或者几种胺的混合溶剂，但是优选使用MDEA溶剂。
5.根据权利要求1所述的捕获方法，其特征在于，所述的叔胺水溶液的质量比为10-40wt％。
6.根据权利要求1所述的捕获方法，其特征在于，所述的包含CO2的气体是燃煤电厂排放的烟道气，CO2含量为10-20vol％，N2含量为85-90vol％。
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