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化学进展 2022, Vol. 34 Issue (7): 1509-1523 DOI: 10.7536/PC220347 前一篇   后一篇

• 综述 •

离子液体的凝聚态化学研究

刘亚伟, 张晓春, 董坤, 张锁江*()   

  1. 离子液体清洁过程北京市重点实验室 中国科学院绿色过程与工程重点实验室 多相复杂系统国家重点实验室 中国科学院过程工程研究所 北京 100190
  • 收稿日期:2022-04-01 修回日期:2022-05-06 出版日期:2022-07-24 发布日期:2022-06-24
  • 通讯作者: 张锁江
  • 基金资助:
    国家自然科学基金项目(21978293); 国家自然科学基金项目(21878296); 北京市自然科学基金项目(2202051)
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Research of Condensed Matter Chemistry on Ionic Liquids

Yawei Liu, Xiaochun Zhang, Kun Dong, Suojiang Zhang()   

  1. Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences,Beijing 100190, China
  • Received:2022-04-01 Revised:2022-05-06 Online:2022-07-24 Published:2022-06-24
  • Contact: Suojiang Zhang
  • Supported by:
    National Natural Science Foundation of China(21978293); National Natural Science Foundation of China(21878296); Beijing Municipal Natural Science Foundation(2202051)

离子液体是可以替代传统溶剂实现高效、低碳、清洁、循环新过程新技术的新型溶剂,在完成“双碳”目标中具有重要的应用价值。同时,离子液体是一种典型的“软凝聚态物质(软物质)”,对它的认识和应用依赖于对其内部多尺度微观结构的研究,这需要以“凝聚态化学”的思想作为未来的研究方向,即对离子液体体系的组成、结构、性质、功能及它们之间的内在关系进行多层次的研究,进而实现对实际应用体系中传递过程和反应过程的调控。在本文中,我们以“凝聚态化学”的视角简要综述了对离子液体的研究。首先介绍了离子液体的化学结构和物理性质,指出理解离子液体性质的变化必须要研究其内部的结构。然后,我们介绍了离子液体从分子层面到纳微尺度的结构,包括离子对、氢键、氢键网络、团簇、界面结构和纳米限域结构。最后,我们对离子液体“凝聚态化学”研究的未来进行了展望。

关键词： 离子液体, 凝聚态化学, 氢键, 团簇, 界面, 纳米限域

Ionic liquids are new solvents that can replace traditional solvents to achieve efficient, low-carbon, clean, recycling, novel processes and technologies, and have important application values in completing the “double carbon” goal. Meanwhile, ionic liquids are a kind of typical “soft condensed matter (soft matter)”, and their fundamental understandings and applications strongly depend on the study of their inner multi-scale microstructures, which requires the idea of “condensed matter chemistry” as the future research direction, that is, performing multi-level studies on the composition, structures, properties, functions and their relationships, and thus to regulate the transport and reaction processes in the real application systems. In this paper, we briefly review the research on ionic liquids from the perspective of “condensed matter chemistry”. At first, we introduce the chemical structures and physicochemical properties of ionic liquids, pointing out that it is necessary to study their inner structures to understand the changes in these properties. We then introduce the structures of ionic liquids from the molecular level to the nano-/micro-scale, including ion pairs, hydrogen bonds, hydrogen bond networks, clusters, interfacial structures, and nano-confined structures. Finally, the future of “condensed matter chemistry” research on ionic liquids is discussed.

Contents

1 Introduction

2 Chemical structure and physicochemical properties of ionic liquids

3 Ion pairs

4 Hydrogen bonds and Hydrogen bond networks

5 Clusters of ionic liquids

6 Interfacial ionic liquid

7 Nano-confined structures

8 Conclusion and outlook

Key words: ionic liquid, condensed matter chemistry, hydrogen bond, cluster, interface, nano-confinement
()
图1 典型离子液体阳离子和阴离子的化学结构,R代表烷基链,亦可被其他基团取代,如烯烃、卤素等
Fig. 1 The chemical structure of cations and anions of typical ionic liquids. R stands for alkyl chains which can also be replaced by other groups, such as olefins, halogens, etc.
图2 阳离子-阴离子对的 (a) 形成, (b) 稳定和 (c) 解离示意图[62]
Fig. 2 Schematic diagram of (a) formation, (b) stabilization and (c) dissociation of cationic-anion pairs[62]. Copyright 2020 American Chemical Society.
图3 离子液体中各种类型的氢键[80]
Fig. 3 Various types of hydrogen bonds in ionic liquids[80]. Copyright 2022 American Chemical Society
图4 Z键和氢键网络。(a) 离子液体晶体中的锯齿状结构[80];(b) [C2mim][BF4]中的氢键网络[75]
Fig. 4 Z bonds and hydrogen bond network. (a) The zigzag configurations in different crystal ionic liquids[80]. Copyright 2022 American Chemical Society. (b) Hydrogen bond networks in [C2mim][BF4][75]. Copyright 2012 American Chemical Society
图5 离子液体团簇。(a) 具有不同长度烷基链的咪唑类离子液体的结构,红色和绿色分别表述离子液体极性和非极性聚集区域[87];(b) 不同含水量的[C8mim][NO3]水溶液的结构, x H 2 O为水分子的摩尔分数,黄色和红色分别表述极性和非极性聚集区域,蓝色为水[93]。(c) [C12mim][Br]在水溶液中形成囊泡的过程, t为时间,绿色为[C12mim]+离子,品红色为水[94]
Fig. 5 Clusters of ionic liquid system. (a) Structures of imidazole ionic liquids with different alkyl chains, red and green represent polar and non-polar aggregation regions of ionic liquid, respectively[87]. Copyright 2006 American Chemical Society. (b) Structures of [C8mim][NO3] aqueous solutions with different water content, x H 2 O is the molar fraction of water molecules, yellow and red represent polar and non-polar aggregation regions, respectively, and blue is water[93]. Copyright 2007 American Chemical Society. (c) The formation process of [C12mim][Br] vesicle in the aqueous solution, t is time, green is [C12mim]+ ion, magenta is water[94]. Copyright 2016 American Chemical Society
图6 不同浓度[C12mim][Br]在水溶液中团簇结构的透射电子显微镜图和分子模拟快照[95,96]
Fig. 6 TEM images and molecular simulation snapshots for clusters of [C12mim][Br] in aqueous solutions with different concentrations[95,96]. Copyright 2013 Royal Society of Chemistry. Copyright 2020 Elsevier
图7 离子液体的气-液/固-液界面。(a) 真空中具有不同长度烷基链的[Cnmim][NO3]层密度分布及模拟快照[86,103];(b) 带负电云母表面[Cnmim][TFSI]的密度分布和表面附近[C8mim][TFSI]的模拟快照[104]
Fig. 7 Gas-liquid/solid-liquid interfaces of ionic liquids. (a) The density profiles and a typical snapshot for slabs of [Cnmim][NO3] with different alkyl chains in the vacuum[86,103]. Copyright 2007 American Chemical Society. Copyright 2008 American Chemical Society. (b) The density profiles of [Cnmim][TFSI] on negatively charged mica surface and the snapshots of [C8mim][TFSI] near the surface[104]. Copyright 2012 Wiley
图8 电极表面的离子液体结构和金属表面超薄离子液体膜。(a) 离子液体双电层结构随电极表面负电量的变化及过程中界面阳离子有序结构的变化[113,115]。(b) 不同金属表面超薄离子液体膜的有序/无序结构[117⇓⇓~120]
Fig. 8 Ionic liquids on electrodes and ultra-thin ionic liquids films on metal surfaces. (a) The changes of the ionic liquid EDL structures with the number of negative charges on the electrodes and the changes of ordered structures of interfacial cations[113,115]. Copyright 2011 American Physical Society. Copyright 2015 Wiley. (b) Ordered/disordered structures of ultra-thin ionic liquid films on different metal surfaces[117⇓⇓~120]. Copyright 2020 Taylor & Francis. Copyright 2013 Beilstein Institute. Copyright 2020 American Chemical Society. Copyright 2020 American Chemical Society
图9 纳米限域空间内的离子液体。(a) 不同直径( D)单壁纳米管中的[Ch][ZnCl3][124]。(b) 不同直径的多壁碳纳米管中的[C4mim][PF6][125]。(c) 不同间距( H)的石墨烯片层中的[C2mim][TFSI][126]。(d) 两种MOF材料中的[C2mim][SCN],上图黑色区域显示孔道的连通性[127]
Fig. 9 Ionic liquids in different nano-confined spaces. (a) [Ch][ZnCl3] confined in single-wall nanotubes of different diameters ( D)[124]. Copyright 2009 American Chemical Society. (b) [C4mim][PF6] confined in multi-wall carbon nanotubes of different diameters[125]. Copyright 2010 American Chemical Society. (c) [C2mim] [TFSI] confined two graphene sheets of different spacing distances[126]. Copyright 2019 Royal Society of Chemistry. (d) [C2mim] [SCN] confined in the two MOFs. The black areas in top figures show the connectivity of nanochannels in the MOFs[127]. Copyright 2018 American Chemical Society
图10 限域离子液体的氢键。(a) [C4mim][PF6]在 D = 1.94 n m碳纳米管中平均氢键随温度的变[128]。(b) [C2mim][TFSI]在石墨烯片层中平均氢键随间距的变化[126]
Fig. 10 Hydrogen bonds in nano-confined ionic liquids. (a) The average number of hydrogen bonds as a function of the temperature in [C4mim][PF6] confined in the carbon nanotube of D = 1.94 nm[128]. Copyright 2011 American Chemical Society. (b) The average number of hydrogen bonds as a function of the spacing distance in [C2mim][TFSI] confined in two graphene sheets[126]. Copyright 2019 Royal Society of Chemistry
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摘要

离子液体的凝聚态化学研究