Controlling phase separation behavior of thermo-responsive ionic liquids through the directed distribution of anionic charge

Controlling phase separation behavior of thermo-responsive ionic liquids through the directed distribution of anionic charge
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DOI:
10.1016/j.molliq.2022.119401
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发表时间:
2022-05
影响因子:
6
通讯作者:
Eva M. Gulotty;Sidharth Sanadhya;Zachary D. Tucker;Saeed S. Moghaddam;B. Ashfeld
Eva M. Gulotty;Sidharth Sanadhya;Zachary D. Tucker;Saeed S. Moghaddam;B. Ashfeld
中科院分区:
化学2区
文献类型:
--
作者:
Eva M. Gulotty;Sidharth Sanadhya;Zachary D. Tucker;Saeed S. Moghaddam;B. Ashfeld

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温敏离子液体(TR-ILs)是一种具有动态物理性质的室温液态盐电解质,被誉为解决能量储存和材料分离效率低下的潜在解决方案。这种潜力受到TR-IL相分离对化学结构的敏感性的阻碍。一个准确的评估离子结构对分子键合的影响是合理的设计所需的键合变化转化为散装材料的行为。我们系统地修改TR-IL的结构,表现出无论是低临界溶解温度(LCST)或上临界溶解温度(UCST)相分离,以隔离特定类型的键合对八个四丁基苯甲酸盐衍生的IL的效果,通过COSMO-RS σ分布分析和变温(VT)1H NMR。我们的研究结果表明,除了氢键之外,阳离子构象灵活性、官能团可用性、阳离子-阴离子配位强度和氢键的方向性在控制IL相分离行为中起着关键作用。All rights reserved.
Thermoresponsive ionic liquids (TR-ILs) are room temperature liquid salt electrolytes with dynamic physical properties which have been hailed as potential solutions to inefficiencies in energy storage and material separations. That potential is hindered by the sensitivity of TR-IL phase separation to chemical structure. An accurate assessment of the effect of ion structure on molecular bonding is required for rational design as bonding changes translate to bulk material behavior. We systematically modify the structure of TR-ILs which exhibit either lower critical solution temperature (LCST) or upper critical solution temperature (UCST) phase separation to isolate the effect of specific types of bonding on eight tetrabutylphosphonium benzoate derived ILs through COSMO-RS sigma profile analysis and variable temperature (VT)1H NMR. Our results reveal that in addition to Hydrogen bonding, cation conformational flexibility, functional group availability, cation–anion coordination strength and directionality of hydrogen bonds play key roles in governing the IL phase separation behavior.© 2017 Elsevier Inc. All rights reserved.