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Cationic clustering influences the phase behaviour of ionic liquids
Thomas Niemann1, Dimitri Zaitsau1, Anne Strate1
1Universität Rostock, Institut für Chemie, Abteilung für Physikalische Chemie, Dr. -Lorenz-Weg 2, 18059, Rostock, Germany.
Scientific Reports
|October 5, 2018
Summary
Like-charged ions in ionic liquids can attract via hydrogen bonding, forming clusters. This challenges conventional electrostatics and influences material properties, enabling control over glass formation and crystallization.
Area of Science:
- Physical Chemistry
- Materials Science
- Supramolecular Chemistry
Background:
- Conventional electrostatic principles dictate that like charges repel.
- Recent studies challenge this for ionic liquids (ILs), showing like-charged ions can attract.
- Cooperative hydrogen bonding is proposed as a mechanism to overcome electrostatic repulsion in ILs.
Purpose of the Study:
- To establish design principles for forming like-charged ion clusters in ionic liquids.
- To investigate the influence of charge delocalization on ion clustering.
- To explore the impact of these clusters on the physical properties of ionic liquids, specifically glass formation and crystallization.
Main Methods:
- Synthesis and characterization of ionic liquids with hydroxyethyl-functionalized cations and a common hydrophobic anion.
- Utilizing differential scanning calorimetry (DSC) to observe glass transition temperatures and phase transitions.
- Employing infrared (IR) spectroscopy to analyze hydrogen bonding and cluster formation.
Main Results:
- Demonstrated that delocalization of positive charge on cations promotes the formation of hydrogen-bonded cationic clusters.
- Showed that localized charges favor conventional cation-anion interactions.
- Observed that ionic liquids containing cationic clusters exhibit enhanced supercooling and glass-forming abilities compared to those forming ion pairs.
Conclusions:
- The formation of hydrogen-bonded cationic clusters in ionic liquids is controllable via cation design, specifically charge delocalization.
- These clusters significantly influence the macroscopic properties of ionic liquids, offering a new route to control glass formation and crystallization.
- This work opens avenues for designing novel ionic liquids with tailored thermal properties for advanced applications.
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