International Tomography Center SB RAS, Institutskaya Street 3a, 630090 Novosibirsk, Russia.
Boreskov Institute of Catalysis SB RAS, Lavrentiev Avenue 5, 630090 Novosibirsk, Russia.
Molecules. 2021 Sep 26;26(19):5828. doi: 10.3390/molecules26195828.
Ionic liquid (IL) glasses have recently drawn much interest as unusual media with unique physicochemical properties. In particular, anomalous suppression of molecular mobility in imidazolium IL glasses vs. increasing temperature was evidenced by pulse Electron Paramagnetic Resonance (EPR) spectroscopy. Although such behavior has been proven to originate from dynamics of alkyl chains of IL cations, the role of electron spin relaxation induced by surrounding protons still remains unclear. In this work we synthesized two deuterated imidazolium-based ILs to reduce electron-nuclear couplings between radical probe and alkyl chains of IL, and investigated molecular mobility in these glasses. The obtained trends were found closely similar for deuterated and protonated analogs, thus excluding the relaxation-induced artifacts and reliably demonstrating structural grounds of the observed anomalies in heterogeneous IL glasses.
离子液体（IL）玻璃最近作为具有独特物理化学性质的非常规介质引起了广泛关注。特别是，通过脉冲电子顺磁共振（EPR）光谱证明了在咪唑基 IL 玻璃中，分子迁移率随温度升高而异常抑制。尽管这种行为已被证明源自 IL 阳离子的烷基链的动力学，但周围质子诱导的电子自旋弛豫的作用仍不清楚。在这项工作中，我们合成了两种氘代咪唑基 IL，以减少自由基探针与 IL 烷基链之间的电子-核偶联，并研究了这些玻璃中的分子迁移率。对于氘代和质子化类似物，获得的趋势非常相似，因此排除了弛豫诱导的假象，并可靠地证明了在非均相 IL 玻璃中观察到的异常的结构基础。
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