Understanding the Liquid Structure in Mixtures of Ionic Liquids with Semiperfluoroalkyl or Alkyl Chains.
Understanding the Liquid Structure in Mixtures of Ionic Liquids with Semiperfluoroalkyl or Alkyl Chains.
复制标题
DOI：
10.1021/acs.jpcb.3c02647
复制
发表时间：
2023-08-24
影响因子：
3.3
通讯作者：
Slattery, John M.
中科院分区：
文献类型：
--
作者：
Elstone, Naomi S.;Shimizu, Karina;Shaw, Emily V.;Lane, Paul D.;D'Andrea, Luciïa;Deme, Bruno;Mahmoudi, Najet;Rogers, Sarah E.;Youngs, Sarah;Costen, Matthew L.;McKendrick, Kenneth G.;Lopes, Jose Canongia N.;Bruce, Duncan W.;Slattery, John M.
通过混合离子液体（IL），可以微调它们的本体和界面结构。这改变了它们的物理性质和溶剂化行为，并且是制备IL集合的简单方法，其性质可以被调节以优化特定应用。在这项研究中，全氟化和烷基化离子液体的混合物已经制备，和组合物，性能和纳米结构之间的联系进行了研究。这些不同类别的离子液体在其链的柔性和极化性方面有很大差异。因此，通过混合可获得一系列有用的结构和物理性质变化，这将扩大在迄今为止受到相对较少关注的领域中可用的IL混合物的库。在本文提供的实验中，制备了1-甲基-3-辛基咪唑鎓双（三氟甲基磺酰基）酰亚胺[C8 MIM][Tf 2N]和1-（1H，1H，2 H，2 H-全氟辛基）-3-甲基咪唑鎓双（三氟甲基磺酰基）酰亚胺[C8 MIM-F13][Tf 2N]的混合物的物理性质和本体结构。使用小角X射线和中子散射（SAXS和SANS，分别）实验结合原子分子动力学模拟和密度和粘度的测量相结合的散装液体结构进行了研究。我们观察到，添加[C8 MIM-F13][Tf 2N]到[C8 MIM][Tf 2N]引起IL混合物的纳米结构的变化，其取决于组成，使得观察到特征短程相关性的变化作为组成的函数。因此，虽然与非极性区域（极性非极性峰-PNPP）相关的长度尺度随着混合物中[C8 MIM-F13][Tf 2N]的比例而增加，但可能令人惊讶地考虑到氟碳链的更大体积，电荷有序峰的长度尺度减小。有趣的是，对接触峰的考虑表明，其起源既在直接阴离子···阳离子接触长度尺度中，也在附加到咪唑鎓阳离子的链的性质（因此体积）中。
By mixing ionic liquids (ILs), it is possible to fine-tune their bulk and interfacial structure. This alters their physical properties and solvation behavior and is a simple way to prepare a collection of ILs whose properties can be tuned to optimize a specific application. In this study, mixtures of perfluorinated and alkylated ILs have been prepared, and links between composition, properties, and nanostructure have been investigated. These different classes of ILs vary substantially in the flexibility and polarizability of their chains. Thus, a range of useful structural and physical property variations are accessible through mixing that will expand the library of IL mixtures available in an area that to this point has received relatively little attention. In the experiments presented herein, the physical properties and bulk structure of mixtures of 1-methyl-3-octylimidazolium bis(trifluoromethylsulfonyl)imide [C8MIM][Tf2N] and 1-(1H,1H,2H,2H-perfluorooctyl)-3-methylimidazolium bis(trifluoromethylsulfonyl)imide [C8MIM-F13][Tf2N] have been prepared. The bulk liquid structure was investigated using a combination of small-angle X-ray and neutron scattering (SAXS and SANS, respectively) experiments in combination with atomistic molecular dynamics simulations and the measurement of density and viscosity. We observed that the addition of [C8MIM-F13][Tf2N] to [C8MIM][Tf2N] causes changes in the nanostructure of the IL mixtures that are dependent on composition so that variation in the characteristic short-range correlations is observed as a function of composition. Thus, while the length scales associated with the apolar regions (polar non-polar peak—PNPP) increase with the proportion of [C8MIM-F13][Tf2N] in the mixtures, perhaps surprisingly given the greater volume of the fluorocarbon chains, the length scale of the charge-ordering peak decreases. Interestingly, consideration of the contact peak shows that its origins are both in the direct anion···cation contact length scale and the nature (and hence volume) of the chains appended to the imidazolium cation.
登录
查看更多内容
DOI：
10.1524/zpch.2006.220.10.1377
发表时间：
2006-01-01
影响因子：
2.5
作者：
Endres, Frank;El Abedin, Sherif Zein;Borissenko, Natalia
通讯作者：
Borissenko, Natalia
影响因子：
--
作者：
GILMOUR, JB;ZWICKER, JO;SCOTT, RL
通讯作者：
SCOTT, RL
影响因子：
4.9
作者：
Kashyap, Hemant K.;Hettige, Jeevapani J.;Margulis, Claudio J.
通讯作者：
Margulis, Claudio J.
影响因子：
6.3
作者：
BERENDSEN, HJC;VANDERSPOEL, D;VANDRUNEN, R
通讯作者：
VANDRUNEN, R
影响因子：
8.4
作者：
Gale, Ella;Wirawan, Remigius H.;Scott, Janet L.
通讯作者：
Scott, Janet L.