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Title: Glass transition dynamics and conductivity scaling in ionic deep eutectic solvents: The case of (acetamide + lithium nitrate/sodium thiocyanate) melts

Abstract

A detailed investigation on the molecular dynamics of ionic deep eutectic solvents (acetamide + lithium nitrate/sodium thiocyanate) is reported. The study was carried out employing dielectric relaxation spectroscopy covering seven decades in frequency (10{sup −1}-10{sup 6} Hz) and in a wide temperature range from 373 K down to 173 K, accessing the dynamic observables both in liquid and glassy state. The dielectric response of the ionic system has been presented in the dynamic window of modulus formalism to understand the conductivity relaxation and its possible connection to the origin of localized motion. Two secondary relaxation processes appear below glass transition temperature. Our findings provide suitable interpretation on the nature of secondary Johari-Goldstein process describing the ion translation and orientation of dipoles in a combined approach using Ngai’s coupling model. A nearly constant loss feature is witnessed at shorter times/lower temperatures. We also discuss the ac conductivity scaling behavior using Summerfield approach and random free energy barrier model which establish the time-temperature superposition principle. These experimental observations have fundamental importance on theoretical elucidation of the conductivity relaxation and glass transition phenomena in molten ionic conductors.

Authors:
; ; ;  [1];  [2];  [3];  [4]
  1. Institute of Physics, University of Silesia, Uniwersytecka 4, 40-007 Katowice (Poland)
  2. (Poland)
  3. Department of Nanomaterial Science and Department of Chemistry, Chiba University, 1-33 Yayoi, Inage-ku, Chiba 263-8522 (Japan)
  4. Department of Chemical, Biological and Macromolecular Sciences, S. N. Bose National Centre for Basic Sciences, JD Block, Sector III, Salt Lake, Kolkata 700098 (India)
Publication Date:
OSTI Identifier:
22415774
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 142; Journal Issue: 18; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ACETAMIDE; COUPLING; DIELECTRIC MATERIALS; EUTECTICS; FREE ENERGY; GLASS; LIQUIDS; LITHIUM NITRATES; MOLECULAR DYNAMICS METHOD; RELAXATION; SODIUM COMPOUNDS; SOLVENTS; SPECTROSCOPY; TEMPERATURE DEPENDENCE; THIOCYANATES; TRANSITION TEMPERATURE

Citation Formats

Tripathy, Satya N., E-mail: satyanarayantripathy@gmail.com, Wojnarowska, Zaneta, Knapik, Justyna, Paluch, Marian, Silesian Center for Education and Interdisciplinary Research, 75 Pulku Piechoty 1A, 41-500 Chorzow, Shirota, Hideaki, and Biswas, Ranjit. Glass transition dynamics and conductivity scaling in ionic deep eutectic solvents: The case of (acetamide + lithium nitrate/sodium thiocyanate) melts. United States: N. p., 2015. Web. doi:10.1063/1.4919946.
Tripathy, Satya N., E-mail: satyanarayantripathy@gmail.com, Wojnarowska, Zaneta, Knapik, Justyna, Paluch, Marian, Silesian Center for Education and Interdisciplinary Research, 75 Pulku Piechoty 1A, 41-500 Chorzow, Shirota, Hideaki, & Biswas, Ranjit. Glass transition dynamics and conductivity scaling in ionic deep eutectic solvents: The case of (acetamide + lithium nitrate/sodium thiocyanate) melts. United States. doi:10.1063/1.4919946.
Tripathy, Satya N., E-mail: satyanarayantripathy@gmail.com, Wojnarowska, Zaneta, Knapik, Justyna, Paluch, Marian, Silesian Center for Education and Interdisciplinary Research, 75 Pulku Piechoty 1A, 41-500 Chorzow, Shirota, Hideaki, and Biswas, Ranjit. Thu . "Glass transition dynamics and conductivity scaling in ionic deep eutectic solvents: The case of (acetamide + lithium nitrate/sodium thiocyanate) melts". United States. doi:10.1063/1.4919946.
@article{osti_22415774,
title = {Glass transition dynamics and conductivity scaling in ionic deep eutectic solvents: The case of (acetamide + lithium nitrate/sodium thiocyanate) melts},
author = {Tripathy, Satya N., E-mail: satyanarayantripathy@gmail.com and Wojnarowska, Zaneta and Knapik, Justyna and Paluch, Marian and Silesian Center for Education and Interdisciplinary Research, 75 Pulku Piechoty 1A, 41-500 Chorzow and Shirota, Hideaki and Biswas, Ranjit},
abstractNote = {A detailed investigation on the molecular dynamics of ionic deep eutectic solvents (acetamide + lithium nitrate/sodium thiocyanate) is reported. The study was carried out employing dielectric relaxation spectroscopy covering seven decades in frequency (10{sup −1}-10{sup 6} Hz) and in a wide temperature range from 373 K down to 173 K, accessing the dynamic observables both in liquid and glassy state. The dielectric response of the ionic system has been presented in the dynamic window of modulus formalism to understand the conductivity relaxation and its possible connection to the origin of localized motion. Two secondary relaxation processes appear below glass transition temperature. Our findings provide suitable interpretation on the nature of secondary Johari-Goldstein process describing the ion translation and orientation of dipoles in a combined approach using Ngai’s coupling model. A nearly constant loss feature is witnessed at shorter times/lower temperatures. We also discuss the ac conductivity scaling behavior using Summerfield approach and random free energy barrier model which establish the time-temperature superposition principle. These experimental observations have fundamental importance on theoretical elucidation of the conductivity relaxation and glass transition phenomena in molten ionic conductors.},
doi = {10.1063/1.4919946},
journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 18,
volume = 142,
place = {United States},
year = {2015},
month = {5}
}