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增加阳离子离子对称性可降低薄膜中离子液体的有序性。

Increasing Cation Ion Symmetry Reduces Ionic Liquid Ordering in Thin Films.

作者信息

Van Den Top Michael Blake, Horvath Andrew, Koutsoukos Spyridon, Philippi Frederik, Rauber Daniel, Welton Tom, Shaw Scott K

机构信息

Department of Chemistry, University of Iowa, Iowa, Iowa 52242, United States.

Department of Chemistry, Imperial College, London SW7 2AZ, U.K.

出版信息

J Phys Chem B. 2024 Nov 14;128(45):11251-11257. doi: 10.1021/acs.jpcb.4c04413. Epub 2024 Nov 5.

DOI:10.1021/acs.jpcb.4c04413
PMID:39500513
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11571225/
Abstract

Ionic liquids have been shown to form extended ordered structures near surfaces and in bulk. Identifying fundamental driving force(s) for this organization has been elusive. In this paper, we test a hypothesis that the ionic liquid asymmetry, inherent in many of the IL formulations to frustrate crystallization, is a significant contributor to the observed ordering. We have carried out measurements to track the ordering of ionic liquids composed of "spherical" cations, namely, tetraoctylphosphonium ([P8888]) and tetra(propoxymethyl)phosphonium [P(3O1)4] paired with tetracyanoborate anion [B(CN)4]. Analysis of the infrared signatures for films of these ionic liquids shows very little evidence of ordered structures. These liquids instead remain in a more isotropic environment even when confined to volumes of few micrometer dimensions.

摘要

离子液体已被证明在表面附近和本体中会形成扩展的有序结构。确定这种组织的基本驱动力一直难以捉摸。在本文中，我们检验了一个假设，即许多离子液体配方中固有的离子液体不对称性（这会阻碍结晶）是观察到的有序性的一个重要因素。我们进行了测量，以追踪由“球形”阳离子（即四辛基鏻（[P8888]）和四（丙氧基甲基）鏻[P(3O1)4]）与四氰基硼酸根阴离子[B(CN)4]组成的离子液体的有序化过程。对这些离子液体薄膜的红外特征分析表明，几乎没有有序结构的证据。相反，即使被限制在几微米尺寸的体积内，这些液体仍处于更各向同性的环境中。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/f6a35690b81f/jp4c04413_0010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/5fb02abd0f73/jp4c04413_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/478886bfd25c/jp4c04413_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/b8c1fd802936/jp4c04413_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/10ea6d9d9e0a/jp4c04413_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/d0549368c3d9/jp4c04413_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/ece503229a08/jp4c04413_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/a4e0cdaed57b/jp4c04413_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/b44ab6f531bd/jp4c04413_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/6e581035ba35/jp4c04413_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/f6a35690b81f/jp4c04413_0010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/5fb02abd0f73/jp4c04413_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/478886bfd25c/jp4c04413_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/b8c1fd802936/jp4c04413_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/10ea6d9d9e0a/jp4c04413_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/d0549368c3d9/jp4c04413_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/ece503229a08/jp4c04413_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/a4e0cdaed57b/jp4c04413_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/b44ab6f531bd/jp4c04413_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/6e581035ba35/jp4c04413_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/67cd/11571225/f6a35690b81f/jp4c04413_0010.jpg

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本文引用的文献

1
Attraction between Like Charged Ions in Ionic Liquids: Unveiling the Enigma of Tetracyanoborate Anions.离子液体中同电荷离子间的吸引力：揭开四氰硼酸根阴离子之谜
J Phys Chem Lett. 2024 Jan 11;15(1):248-253. doi: 10.1021/acs.jpclett.3c02983. Epub 2024 Jan 2.
2
Room temperature ionic liquids with two symmetric ions.含有两个对称离子的室温离子液体。
Chem Sci. 2023 Sep 8;14(37):10340-10346. doi: 10.1039/d3sc03240j. eCollection 2023 Sep 27.
3
Pressing matter: why are ionic liquids so viscous?紧迫问题：离子液体为何如此黏稠？
Chem Sci. 2022 Feb 8;13(9):2735-2743. doi: 10.1039/d1sc06857a. eCollection 2022 Mar 2.
4
Near-Wall Molecular Ordering of Dilute Ionic Liquids.稀离子液体的近壁分子排列
J Phys Chem C Nanomater Interfaces. 2017 Aug 31;121(34):18593-18597. doi: 10.1021/acs.jpcc.7b04843. Epub 2017 Aug 8.
5
Communication: Stiff and soft nano-environments and the "Octopus Effect" are the crux of ionic liquid structural and dynamical heterogeneity.通讯：刚性和柔性纳环境与“章鱼效应”是离子液体结构和动力学不均匀性的关键。
J Chem Phys. 2017 Aug 14;147(6):061102. doi: 10.1063/1.4990666.
6
When Like Charged Ions Attract in Ionic Liquids: Controlling the Formation of Cationic Clusters by the Interaction Strength of the Counterions.当离子液体中的同电荷离子相互吸引时：通过抗衡离子的相互作用强度控制阳离子簇的形成。
Angew Chem Int Ed Engl. 2017 Jan 9;56(2):496-500. doi: 10.1002/anie.201609799. Epub 2016 Dec 19.
7
Long-Range Ordering of Ionic Liquid Fluid Films.离子液体流体膜的长程有序。
Langmuir. 2016 May 24;32(20):5147-54. doi: 10.1021/acs.langmuir.6b00304. Epub 2016 May 10.
8
Modern Room Temperature Ionic Liquids, a Simple Guide to Understanding Their Structure and How It May Relate to Dynamics.现代室温离子液体：理解其结构及其与动力学关系的简易指南
J Phys Chem B. 2015 Oct 8;119(40):12727-40. doi: 10.1021/acs.jpcb.5b05506. Epub 2015 Aug 10.
9
How does the ionic liquid organizational landscape change when nonpolar cationic alkyl groups are replaced by polar isoelectronic diethers?当非极性阳离子烷基基团被等电子极性二醚取代时，离子液体的组织景观会如何变化？
J Phys Chem B. 2013 Jan 31;117(4):1130-5. doi: 10.1021/jp311032p. Epub 2013 Jan 22.
10
Quantum mechanical continuum solvation models for ionic liquids.量子力学连续溶剂化模型在离子液体中的应用。
J Phys Chem B. 2012 Aug 2;116(30):9122-9. doi: 10.1021/jp304365v. Epub 2012 Jul 13.