Crowhurst Lorna, Falcone Ruben, Lancaster N Llewellyn, Llopis-Mestre Veronica, Welton Tom
Department of Chemistry, Imperial College London, South Kensington Campus, London, SW7 2AZ, UK.
J Org Chem. 2006 Nov 10;71(23):8847-53. doi: 10.1021/jo0615302.
In this paper, we report the effect of ionic liquids on substitution reactions using a variety of anionic nucleophiles. We have combined new studies of the reactivity of polyatomic anions, acetate, trifuoroacetate, cyanide, and thiocyanide, with our previous studies of the halides in [C4C1py][Tf2N], [C4C1py][TfO], and [C4C1im][Tf2N] (where [C4C1im]+ is 1-butyl-3-methylimidazolium and [C4C1py]+ is 1-butyl-1-methylpyrrolidinium) and compared their reactivities, k2, to the same reactions in the molecular solvents dichloromethane, dimethylsulfoxide, and methanol. The Kamlet-Taft solvent descriptors (alpha, beta, pi) have been used to analyze the rates of the reactions, which were found to have a strong inverse dependency on the alpha value of the solvent. This result is attributed to the ability of the solvent to hydrogen bond to the nucleophile, so reducing its reactivity. The Eyring activation parameters (DeltaH++ and DeltaS++), while confirming the reaction mechanism, do not offer obvious correlations with the Kamlet-Taft solvent descriptors.
在本文中,我们报告了离子液体对使用多种阴离子亲核试剂的取代反应的影响。我们将对多原子阴离子(乙酸根、三氟乙酸根、氰根和硫氰根)反应活性的新研究与我们之前在[C4C1py][Tf2N]、[C4C1py][TfO]和[C4C1im][Tf2N](其中[C4C1im]+为1-丁基-3-甲基咪唑鎓,[C4C1py]+为1-丁基-1-甲基吡咯烷鎓)中对卤化物的研究相结合,并将它们的反应活性k2与在分子溶剂二氯甲烷、二甲基亚砜和甲醇中相同反应的活性进行了比较。已使用Kamlet-Taft溶剂描述符(α、β、π)来分析反应速率,发现反应速率与溶剂的α值呈强烈的反比关系。该结果归因于溶剂与亲核试剂形成氢键的能力,从而降低了其反应活性。艾林活化参数(ΔH++和ΔS++)虽然证实了反应机理,但与Kamlet-Taft溶剂描述符没有明显相关性。