Heterogenous Dynamics of Diffusive Motion in Organic Ionic Plastic Crystal Studied Using Spin-Spin Relaxation Time: N, N-Diethylpyrrolidinium Bis(fluorosulfonyl)amide

IF 3.3 3区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY

Bulletin of the Chemical Society of Japan Pub Date : 2024-08-19 DOI:10.1093/bulcsj/uoae088

Keiko Nishikawa, Kozo Fujii, Kazuhiko Matsumoto, Hiroshi Abe, Masahiro Yoshizawa-Fujita

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Abstract

The temperature dependences of the spin–spin relaxation times (T2) of 1H and 19F nuclei were measured for N, N-diethylpyrrolidinium bis(fluorosulfonyl)amide with a plastic crystal (PC) phase. In the PC phase, two types of T2 were observed in both 1H and 19F experiments, which was considered to be the appearance of heterogeneous dynamics of diffusive motion. By examining temperature dependences of the T2 values and the existence ratios, the following conclusions were reached. (1) The prepared PC sample was in a polycrystalline state, and each crystallite comprised two phases: the core phase (PC phase) and the surface phase formed to relieve surface stress. (2) The 1H-T2 (19F-T2) values of the two phases differed, and ions in the surface phase were more mobile. The 1H-T2 (19F-T2) values for the two phases increased with temperature rise. In particular, the 1H-T2 (19F-T2) values of the surface phase were smoothly connected to the liquid T2 values. (3) The cations and anions exhibited a cooperative diffusive motion. (4) When the temperature was considerably lower than the melting point, the ratio of the surface phase did not significantly differ from when it first formed. However, it rapidly increased near the melting point and became liquid.

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利用自旋-自旋弛豫时间研究有机离子塑料晶体中扩散运动的异质动力学：N, N-二乙基吡咯烷双（氟磺酰）酰胺

测量了具有塑性晶体（PC）相的 N, N-二乙基吡咯烷双（氟磺酰）酰胺的 1H 和 19F 原子核的自旋-自旋弛豫时间（T2）的温度依赖性。在 PC 相中，1H 和 19F 实验都观察到了两种类型的 T2，这被认为是扩散运动的异质动力学的表现。通过研究 T2 值和存在比的温度相关性，得出了以下结论。(1）制备的 PC 样品处于多晶状态，每个晶粒由两相组成：核心相（PC 相）和为缓解表面应力而形成的表面相。(2) 两相的 1H-T2 (19F-T2) 值不同，表面相中的离子流动性更大。两相的 1H-T2（19F-T2）值随温度升高而增加。尤其是表相的 1H-T2 （19F-T2）值与液相的 T2 值平稳相连。(3) 阳离子和阴离子表现出协同扩散运动。(4) 当温度大大低于熔点时，表面相的比率与最初形成时没有明显差别。然而，当温度接近熔点时，表面相的比例迅速增加并变成液态。

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来源期刊

Bulletin of the Chemical Society of Japan 化学-化学综合

CiteScore

6.40

自引率

5.00%

发文量

194

审稿时长

3-8 weeks

期刊介绍： The Bulletin of the Chemical Society of Japan (BCSJ) is devoted to the publication of scientific research papers in the fields of Theoretical and Physical Chemistry, Analytical and Inorganic Chemistry, Organic and Biological Chemistry, and Applied and Materials Chemistry. BCSJ appears as a monthly journal online and in advance with three kinds of papers (Accounts, Articles, and Short Articles) describing original research. The purpose of BCSJ is to select and publish the most important papers with the broadest significance to the chemistry community in general. The Chemical Society of Japan hopes all visitors will notice the usefulness of our journal and the abundance of topics, and welcomes more submissions from scientists all over the world.