Key Laboratory of Environmental Friendly Function Materials, Ministry of Education, College of Materials Science and Engineering, Huaqiao University, Xiamen 361021, P.R. China.
Dalton Trans. 2019 Feb 12;48(7):2300-2307. doi: 10.1039/c8dt04680h.
In this work, an efficient strategy for improving CO2 capture based on anion-functionalized ionic liquids (ILs) by reducing cation-anion interactions in ILs was reported. The influence of the cationic species on CO2 absorption was investigated using 2-hydroxyl pyridium anions ([2-Op]) as a probe. CO2 capture experiments indicated that the CO2 absorption capacity in [2-Op] anion-based ILs varied from 0.94 to 1.69 mol CO2 per mol IL at 30 °C and 1 atm. Spectroscopic analysis and quantum chemical calculations suggested that the increase of the CO2 absorption capacity may be ascribed to the reduction of the strength of cation-anion interactions in ILs, and stronger cation-anion interactions would make one CO2 site in the [2-Op] anion inactive. Furthermore, the effect of the cation unit on the anion was evidenced by FT-IR spectra, implying that strong interactions between ions may lead to the decrease of the IR absorption wavenumber of hydroxy pyridium and work against CO2 capture. Following this strategy, it was finally found that [Ph-C8eim][2-Op] (Ph-C8eim = 1-N-ethyl-3-N-octyl-2-phenylimidazolium) with weaker cation-anion interactions exhibited a significant increase in the CO2 uptake capacity, and extremely high capacities of 1.69 and 1.83 mol CO2 per mol IL could be achieved at 30 and 20 °C, respectively. The study presented here would be helpful for further designing novel and effective ILs for advancing CO2 capturing performance.
在这项工作中,报道了一种通过降低离子液体中阴阳离子相互作用来提高 CO2 捕集效率的有效策略。采用 2-羟基吡啶鎓阴离子([2-Op])作为探针,研究了阳离子种类对 CO2 吸收的影响。CO2 捕集实验表明,在 30°C 和 1 大气压下,[2-Op]阴离子基 ILs 的 CO2 吸收容量在 0.94 到 1.69 mol CO2/mol IL 之间变化。光谱分析和量子化学计算表明,CO2 吸收容量的增加可能归因于 ILs 中阴阳离子相互作用强度的降低,而更强的阴阳离子相互作用会使[2-Op]阴离子中的一个 CO2 位点失活。此外,FT-IR 光谱证实了阳离子单元对阴离子的影响,这表明离子之间的强相互作用会导致羟基吡啶的 IR 吸收峰数减少,从而不利于 CO2 捕集。根据这一策略,最终发现具有较弱阴阳离子相互作用的[Ph-C8eim][2-Op](Ph-C8eim=1-N-乙基-3-N-辛基-2-苯基咪唑鎓)的 CO2 吸收容量显著增加,在 30°C 和 20°C 下,分别可以达到 1.69 和 1.83 mol CO2/mol IL 的极高容量。本研究有助于进一步设计新型有效的 ILs,以提高 CO2 捕集性能。