A novel Amino Functionalized Ionic Liquid/Organic Solvent with low viscosity for CO2 capture.
A novel Amino Functionalized Ionic Liquid/Organic Solvent with low viscosity for CO2 capture.
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DOI：
10.1021/acs.est.9b06717
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发表时间：
2020-02
影响因子：
11.4
通讯作者：
Fan Liu;Yao Shen;Li Shen;Cheng-Yue Sun;Liang Chen;Qiaoli Wang;Sujing Li;Wei Li
中科院分区：
文献类型：
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作者：
Fan Liu;Yao Shen;Li Shen;Cheng-Yue Sun;Liang Chen;Qiaoli Wang;Sujing Li;Wei Li
为了实现低再生能耗和低粘度，本工作提出了一种新型的氨基官能化离子液体[TEPAH][2-MI]与有机溶剂结合用于CO2捕集。结果表明，[TEPAH][2-MI]/NPA/EG的吸附负荷为1.72 mol·mol-1（28wt%，257 g·L-1），远高于MEA/水，第5次再生后再生效率仍保持在90.7%。吸附前后溶液粘度仅为3.66和7.65 mPa·s，明显低于传统非水吸附剂。通过13 CNMR和量子化学计算，总结了反应机理：CO2首先与[TEPAH]+的氨基通过两性离子化和质子化反应生成氨基甲酸酯，而CO2与[2-MI]-的N原子直接反应生成氨基甲酸酯。然后，其中一些进一步与NPA和EG反应形成碳酸酯。此外，[TEPAH][2-MI]的Nπ和Nτ互变异构体在吸收CO2的过程中可以连续地相互转化。在CO2解吸过程中，氨基甲酸酯和碳酸酯与AFILH+反应分解并直接释放CO2。
To achieve low regeneration energy consumption and viscosity, a novel amino functionalized ionic liquid of [TEPAH][2-MI] combined with organic solvents has been proposed for CO2 capture in this work. The results demonstrated that the absorption loading of [TEPAH][2-MI]/NPA/EG was 1.72 mol·mol-1 (28 wt%, 257 g·L-1), which was much higher than that of MEA/water, and the regeneration efficiency was maintained at 90.7% after the 5th regeneration cycle. The viscosities of the solution were only 3.66 and 7.65 mPa·s before and after absorption, which were significantly lower than that of traditional non-aqueous absorbents. The reaction mechanism investigated via 13C NMR and quantum calculations were summarized that CO2 firstly reacted with the amino group of [TEPAH]+ to form the carbamates through the zwitterion formation and protonation process, while CO2 reacted with the N atom of [2-MI]- to directly form carbamate. Then some of them further reacted with NPA and EG to form the carbonates. Moreover, Nπ and Nτ tautomers of [TEPAH][2-MI] could convert into each other continuously when CO2 was absorbed. During CO2 desorption, the carbamates and carbonates reacted with AFILH+ to decompose and released CO2 directly.