Ion transport and structural dynamics in homologous ammonium and phosphonium-based room temperature ionic liquids

The Journal of Chemical Physics
Philip J GriffinAlexei P Sokolov

Abstract

Charge transport and structural dynamics in a homologous pair of ammonium and phosphonium based room temperature ionic liquids (ILs) have been characterized over a wide temperature range using broadband dielectric spectroscopy and quasi-elastic light scattering spectroscopy. We have found that the ionic conductivity of the phosphonium based IL is significantly enhanced relative to the ammonium homolog, and this increase is primarily a result of a lower glass transition temperature and higher ion mobility. Additionally, these ILs exhibit pronounced secondary relaxations which are strongly influenced by the atomic identity of the cation charge center. While the secondary relaxation in the phosphonium IL has the expected Arrhenius temperature dependence characteristic of local beta relaxations, the corresponding relaxation process in the ammonium IL was found to exhibit a mildly non-Arrhenius temperature dependence in the measured temperature range-indicative of molecular cooperativity. These differences in both local and long-range molecular dynamics are a direct reflection of the subtly different inter-ionic interactions and mesoscale structures found in these homologous ILs.

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Citations

Apr 3, 2016·The Journal of Chemical Physics·Jeevapani J HettigeClaudio J Margulis
Jul 9, 2016·The Journal of Chemical Physics·Philip J GriffinAlexei P Sokolov
Jun 17, 2016·The Journal of Chemical Physics·Thamires A LimaCarlos Giles
Jul 18, 2017·The Journal of Physical Chemistry Letters·Tyler CosbyJoshua Sangoro
Oct 12, 2018·The Journal of Chemical Physics·Fangfang ChenMaria Forsyth
May 21, 2016·Physical Review Letters·L N PatroB Roling
Dec 24, 2017·The Journal of Chemical Physics·Tyler CosbyJoshua Sangoro
Sep 17, 2020·The Journal of Chemical Physics·Elisa SteinrückenMichael Vogel
Oct 12, 2018·The Journal of Chemical Physics·T CosbyJ Sangoro
Jun 24, 2021·Physical Chemistry Chemical Physics : PCCP·Florian PabstThomas Blochowicz
Sep 29, 2019·The Journal of Physical Chemistry Letters·Tyler CosbyJoshua Sangoro
Jun 12, 2019·The Journal of Physical Chemistry. B·Adhip RahmanMd Abu Bin Hasan Susan
Apr 16, 2020·Chemical Reviews·Yong-Lei WangMichael D Fayer

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