College of Environmental Science and Engineering, Guilin University of Technology, Guilin 541004, China.
Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin 541004, China.
Environ Sci Technol. 2020 Dec 15;54(24):16138-16146. doi: 10.1021/acs.est.0c05774. Epub 2020 Nov 25.
To address the problems of the relatively high energy penalty and corrosivity of aqueous biphasic solvents, a novel nonaqueous biphasic solvent composed of 2-((2-aminoethyl)amino)ethanol (AEEA), dimethyl sulfoxide (DMSO), and ,,,,-pentamethyldiethylenetriamine (PMDETA) was proposed for CO capture. With optimization, this novel AEEA-DMSO-PMDETA (A-D-P) biphasic solvent could achieve a high CO loading of 1.75 mol·mol, of which 96.8% of the absorbed CO was enriched in the lower phase with only 49.6% of the total volume. C NMR analysis and quantum calculations revealed that A-D-P could absorb CO to form not only carbamate but also carbamic acid species, which were stabilized by DMSO via hydrogen-bonding interactions. Most products were highly polar and preferred to dissolve in polar DMSO rather than the less polar PMDETA, thus leading to the phase change. The thermodynamics results showed that the heat duty of A-D-P was only 1.66 GJ·ton CO (393.15 K), which was significantly lower than that of the benchmark MEA (3.59 GJ·ton CO) and the reported aqueous biphasic solvents. Moreover, A-D-P presented a noncorrosive behavior to steel after CO saturation, clearly showing its superiority over MEA and the aqueous biphasic solvents. Therefore, with superior properties of energy savings and noncorrosiveness, the A-D-P biphasic solvent could be a promising candidate for CO capture.
为了解决水相双相溶剂能量损耗较高和腐蚀性较强的问题,提出了一种新型非水相双相溶剂,由 2-((2-氨基乙基)氨基)乙醇(AEEA)、二甲基亚砜(DMSO)和 1,4,7,10,13-五氧杂-1,6,9-三氮杂环十五烷(PMDETA)组成,用于 CO 捕集。通过优化,这种新型 AEEA-DMSO-PMDETA(A-D-P)双相溶剂可以实现高达 1.75 mol·mol 的高 CO 负载量,其中 96.8%的吸收 CO 富集在较低相中,仅占总体积的 49.6%。C NMR 分析和量子计算表明,A-D-P 可以吸收 CO 形成不仅是氨基甲酸酯,还有氨基甲酸,它们通过氢键相互作用被 DMSO 稳定。大多数产物具有很高的极性,更倾向于溶解在极性的 DMSO 中,而不是极性较小的 PMDETA 中,从而导致相变化。热力学结果表明,A-D-P 的热负荷仅为 1.66 GJ·ton CO(393.15 K),显著低于基准 MEA(3.59 GJ·ton CO)和报道的水相双相溶剂。此外,A-D-P 在 CO 饱和后对钢表现出非腐蚀性行为,明显优于 MEA 和水相双相溶剂。因此,A-D-P 双相溶剂具有节能和非腐蚀性的优异性能,可能是 CO 捕集的有前途的候选溶剂。