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Title: Water Dynamics in 1-Alkyl-3-methylimidazolium Tetrafluoroborate Ionic Liquids

Abstract

The effects of water concentration and varying alkyl chain length on the dynamics of water in 1-alkyl-3-methylimidazolium tetrafluoroborate room temperature ionic liquids (RTILs) were characterized using two dimensional infrared (2D IR) vibrational echo spectroscopy and polarization-selective IR pump-probe experiments to study the water hydroxyl (OD) stretching mode of dilute HOD in H2O. Three imidazolium cation alkyl chain lengths, ethyl (Emim+), butyl (Bmim+), and decyl (Dmim+), were investigated. Both the Bmim+ and Dmim+ cations have sufficiently long chains that the liquids exhibit polar-apolar segregation, while the Emim+ ionic liquid has no significant apolar aggregation. While the OD absorption spectra were independent of the chain length, the measured reorientation and spectral diffusion dynamics were chain length dependent and tend to slow when the alkyl chain is long enough for polar-apolar segregation. As the water concentration is increased, a water-associated water population forms, absorbing in a new spectral region red-shifted from the isolated, anion-associated, water population. Furthermore, the anion-associated water dynamics are accelerated. At sufficiently high water concentrations, water in all the RTILs experiences similar dynamics, the solvent structures having been fluidized by the addition of water. Here, the water concentration at which the dilute water dynamics changes to fluidized dynamics depends onmore » the alkyl chain length, which determines the extent and ordering of the apolar regions. Increases in both water concentration and alkyl chain length serve to modify the ordering of the RTIL, but with opposite and competing effects on the dissolved water dynamics.« less

Authors:
 [1];  [1];  [1];  [1]
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  1. Stanford Univ., CA (United States)
Publication Date:
Research Org.:
Stanford Univ., CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
OSTI Identifier:
1797789
Grant/Contract Number:  
FG02-84ER13251
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 120; Journal Issue: 44; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 14 SOLAR ENERGY; Hydroxyls; Noncovalent interactions; Solution chemistry; Alkyls; Diffusion

Citation Formats

Giammanco, Chiara H., Kramer, Patrick L., Wong, Daryl B., and Fayer, Michael D. Water Dynamics in 1-Alkyl-3-methylimidazolium Tetrafluoroborate Ionic Liquids. United States: N. p., 2016. Web. doi:10.1021/acs.jpcb.6b08410.
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Giammanco, Chiara H., Kramer, Patrick L., Wong, Daryl B., & Fayer, Michael D. Water Dynamics in 1-Alkyl-3-methylimidazolium Tetrafluoroborate Ionic Liquids. United States. https://doi.org/10.1021/acs.jpcb.6b08410
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Giammanco, Chiara H., Kramer, Patrick L., Wong, Daryl B., and Fayer, Michael D. Tue . "Water Dynamics in 1-Alkyl-3-methylimidazolium Tetrafluoroborate Ionic Liquids". United States. https://doi.org/10.1021/acs.jpcb.6b08410. https://www.osti.gov/servlets/purl/1797789.
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@article{osti_1797789,
title = {Water Dynamics in 1-Alkyl-3-methylimidazolium Tetrafluoroborate Ionic Liquids},
author = {Giammanco, Chiara H. and Kramer, Patrick L. and Wong, Daryl B. and Fayer, Michael D.},
abstractNote = {The effects of water concentration and varying alkyl chain length on the dynamics of water in 1-alkyl-3-methylimidazolium tetrafluoroborate room temperature ionic liquids (RTILs) were characterized using two dimensional infrared (2D IR) vibrational echo spectroscopy and polarization-selective IR pump-probe experiments to study the water hydroxyl (OD) stretching mode of dilute HOD in H2O. Three imidazolium cation alkyl chain lengths, ethyl (Emim+), butyl (Bmim+), and decyl (Dmim+), were investigated. Both the Bmim+ and Dmim+ cations have sufficiently long chains that the liquids exhibit polar-apolar segregation, while the Emim+ ionic liquid has no significant apolar aggregation. While the OD absorption spectra were independent of the chain length, the measured reorientation and spectral diffusion dynamics were chain length dependent and tend to slow when the alkyl chain is long enough for polar-apolar segregation. As the water concentration is increased, a water-associated water population forms, absorbing in a new spectral region red-shifted from the isolated, anion-associated, water population. Furthermore, the anion-associated water dynamics are accelerated. At sufficiently high water concentrations, water in all the RTILs experiences similar dynamics, the solvent structures having been fluidized by the addition of water. Here, the water concentration at which the dilute water dynamics changes to fluidized dynamics depends on the alkyl chain length, which determines the extent and ordering of the apolar regions. Increases in both water concentration and alkyl chain length serve to modify the ordering of the RTIL, but with opposite and competing effects on the dissolved water dynamics.},
doi = {10.1021/acs.jpcb.6b08410},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 44,
volume = 120,
place = {United States},
year = {Tue Oct 11 00:00:00 EDT 2016},
month = {Tue Oct 11 00:00:00 EDT 2016}
}
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https://doi.org/10.1021/acs.jpcb.6b08410
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