State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, China.
J Phys Chem B. 2011 May 26;115(20):6585-91. doi: 10.1021/jp1124074. Epub 2011 May 4.
Task-specific ionic liquids (TSILs) have been experimentally demonstrated to absorb more sulfur dioxide (SO(2)) than normal ILs from gas mixtures with low SO(2) concentrations; however, the differences of SO(2) solubilities in the two kinds of ILs at given temperatures and pressures have not been studied systematically. Moreover, the mechanism of the interaction between SO(2) and ILs still remains unclear. In this work, the solubilities of SO(2) in TSILs (1,1,3,3-tetramethylguanidinium lactate and monoethanolaminium lactate) and normal ILs (1-butyl-3-methylimidazolium tetrafluoroborate and 1-butyl-3-methylimidazolium hexafluorophosphate) were determined. The solubilities of SO(2) are correlated by a modified Redlich-Kwong equation of state (RK EoS). The chemical absorption and physical absorption are differentiated, and the absorption mechanism has been proposed with the aid of the modified RK EoS. SO(2) absorption capacity in TSILs is contributed from both chemical interaction and physical interaction. Two TSIL molecules chemically absorb one SO(2) molecule, and the chemical absorption amount follows the chemical equilibrium. Normal ILs only physically absorb SO(2) following Henry's law. The chemical equilibrium constant, reaction enthalpy, Gibbs energy of reaction, reaction entropy, and Henry's law constant of SO(2) absorbed in ILs have been calculated. The present model can predict SO(2) absorption capacity for capture and SO(2) equilibrium concentration in IL for recovery.
任务特异性离子液体(TSILs)已被实验证明,与普通 ILs 相比,其能够从低浓度 SO2 的混合气体中吸收更多的二氧化硫(SO2);然而,在给定温度和压力下,这两种 ILs 中 SO2 的溶解度差异尚未得到系统研究。此外,SO2 与 ILs 之间的相互作用机制仍不清楚。在这项工作中,测定了 SO2 在 TSILs(1,1,3,3-四甲基胍乳酸盐和单乙醇胺乳酸盐)和普通 ILs(1-丁基-3-甲基咪唑四氟硼酸盐和 1-丁基-3-甲基咪唑六氟磷酸盐)中的溶解度。SO2 的溶解度由修正的 Redlich-Kwong 状态方程(RK EoS)关联。区分了化学吸收和物理吸收,并借助修正的 RK EoS 提出了吸收机制。TSILs 中的 SO2 吸收能力来自化学相互作用和物理相互作用。两个 TSIL 分子化学吸收一个 SO2 分子,化学吸收量遵循化学平衡。普通 ILs 仅根据亨利定律物理吸收 SO2。计算了 IL 中 SO2 的化学平衡常数、反应焓、反应吉布斯自由能、反应熵和亨利定律常数。该模型可用于预测捕获的 SO2 吸收能力和 IL 中 SO2 的平衡浓度。