Combined Experimental and Computational Study on the Structure-Property Relationships of Mono- and Dicationic Imidazolium Ionic Liquids for CO(2) Capture

单阳离子和双阳离子咪唑鎓离子液体结构-性质关系及其对CO(2)捕获性能的实验与计算相结合研究

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Abstract

The present study investigates the potential of dicationic ionic liquids (DILs) and monocationic ionic liquids (MoIL), with and without metal in the anion, for CO(2) capture applications. The structures of the samples were confirmed by FTIR, (1)H NMR spectroscopy, and Raman spectroscopy, while their physicochemical properties, density, viscosity, and thermal stability were evaluated. A series of computational simulations were conducted by using density functional theory (M11/def2-TZVP) to ascertain the multiplicity of the ground state of the magnetic anion [FeCl(4)](-). These simulations determined the multiplicity to be a sextet and furthermore identified the trans conformation as the most energetically favorable for cation [E(MIM)(2)](2+). This finding demonstrates a correlation between the structural conformations and the experimental Raman spectra. The findings of CO(2) sorption and kinetic tests, conducted under postcombustion conditions (40 °C, 4 bar), indicated that DILs exhibited superior performance in comparison to MoILs. The DIL [E(MIM)(2)][2Cl] exhibited the highest sorption capacity (110.20 μmol/g), which is almost three times higher than that of the best MoIL (BMIM FeCl(4)). These enhancements can be ascribed to reduced viscosities and an augmented number of active interaction sites in the dicationic structures. Furthermore, [E(MIM)(2)][2Cl] exhibited a high degree of selectivity for CO(2) over N(2) and demonstrated stability over five recycling cycles, suggesting the potential of DILs as candidates for the development of CO(2) capture technologies.

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