Combining results from impedance spectroscopy and oscillatory shear rheology, the present work focuses on the relation between the mass and charge flows and on how these are affected by the H-bonding in viscous ionic liquids (ILs). In particular, we compare the relaxational behaviors of the paradigmatic IL 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (EMIM-TFSI) and its OH-functionalized counterpart 1-(2-hydroxyethyl)-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (OHEMIM-TFSI). Our results and their analysis demonstrate that the presence of cationic OH-groups bears a strong impact on the overall dynamics of OHEMIM-TFSI, although no signatures of suprastructural relaxation modes could be identified in their dielectric and mechanical responses. To check whether at the origin of this strong variation is the H-bonding or merely the difference between the corresponding cation sizes (controlling both the hydrodynamic volume and the inter-charge distance), the present study includes 1-propyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide (PMIM-TFSI), mixtures of EMIM-TFSI and PMIM-TFSI with lithium bis(trifluoromethylsulfonyl)imide (Li-TFSI), and mixtures of OHEMIM-TFSI with PMIM-TFSI. Their investigation clearly reveals that the dynamical changes induced by H-bonding are significantly larger than those that can be attributed to the change in the ion size. Moreover, in the mixtures of OHEMIM-TFSI with PMIM-TFSI, a dilution of the OH-groups leads to strong deviations from ideal mixing behavior, thus highlighting the common phenomenological ground of hydroxy-functionalized ILs and other H-bonded liquids.

中文翻译：

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通过氢键调节咪唑基离子液体的动力学。I.粘性制度

结合阻抗谱和振荡剪切流变学的结果，本工作着重于质量和电荷流之间的关系，以及粘滞性离子液体（ILs）中的H键如何影响电荷流和电荷流。特别是，我们比较了范式IL 1-乙基-3-甲基咪唑双（三氟甲基磺酰基）酰亚胺（EMIM-TFSI）和其OH-官能化的对应物1-（2-羟乙基）-3-甲基咪唑双（三氟甲基磺酰基）的弛豫行为。酰亚胺（OHEMIM-TFSI）。我们的结果和他们的分析表明，阳离子OH-基团的存在对OHEMIM-TFSI的整体动力学具有强烈影响，尽管在其介电和机械响应中未发现超结构弛豫模式的特征。为了检查这种强烈变化的根源是氢键还是仅仅是相应阳离子尺寸之间的差异（控制流体动力学体积和电荷间距离），本研究包括1-丙基-3-甲基咪唑鎓双（三氟甲基磺酰基）酰亚胺（PMIM-TFSI），EMIM-TFSI和PMIM-TFSI与双（三氟甲基磺酰基）酰亚胺锂（Li-TFSI）的混合物以及OHEMIM-TFSI与PMIM-TFSI的混合物。他们的研究清楚地表明，由氢键引起的动力学变化远大于可归因于离子尺寸变化的动力学变化。此外，在OHEMIM-TFSI与PMIM-TFSI的混合物中，OH基团的稀释会导致与理想混合行为的强烈偏离，