Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former

Abstract In this paper the relaxation dynamics of ionic glass-former acebutolol hydrochloride (ACB-HCl) is studied as a function of temperature and pressure by using dynamic light scattering and broadband dielectric spectroscopy. These unique experimental data provide the first direct evidence that...

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Autores principales:	Z. Wojnarowska, M. Rams-Baron, J. Knapik-Kowalczuk, A. Połatyńska, M. Pochylski, J. Gapinski, A. Patkowski, P. Wlodarczyk, M. Paluch
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/340efe071e10419eb5a2e39eb4d572d8
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spelling	oai:doaj.org-article:340efe071e10419eb5a2e39eb4d572d82021-12-02T16:05:59ZExperimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former10.1038/s41598-017-07136-52045-2322https://doaj.org/article/340efe071e10419eb5a2e39eb4d572d82017-08-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-07136-5https://doaj.org/toc/2045-2322Abstract In this paper the relaxation dynamics of ionic glass-former acebutolol hydrochloride (ACB-HCl) is studied as a function of temperature and pressure by using dynamic light scattering and broadband dielectric spectroscopy. These unique experimental data provide the first direct evidence that the decoupling between the charge transport and structural relaxation exists in proton conductors over a wide T-P thermodynamic space, with the time scale of structural relaxation being constant at the liquid-glass transition (τα = 1000 s). We demonstrate that the enhanced proton transport, being a combination of intermolecular H+ hopping between cation and anion as well as tautomerization process within amide moiety of ACB molecule, results in a breakdown of the Stokes-Einstein relation at ambient and elevated pressure with the fractional exponent k being pressure dependent. The dT g /dP coefficient, stretching exponent βKWW and dynamic modulus E a /ΔV # were found to be the same regardless of the relaxation processes studied. This is in contrast to the apparent activation volume parameter that is different when charge transport and structural dynamics are considered. These experimental results together with theoretical considerations create new ideas to design efficient proton conductors for potential electrochemical applications.Z. WojnarowskaM. Rams-BaronJ. Knapik-KowalczukA. PołatyńskaM. PochylskiJ. GapinskiA. PatkowskiP. WlodarczykM. PaluchNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-8 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Z. Wojnarowska M. Rams-Baron J. Knapik-Kowalczuk A. Połatyńska M. Pochylski J. Gapinski A. Patkowski P. Wlodarczyk M. Paluch Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
description	Abstract In this paper the relaxation dynamics of ionic glass-former acebutolol hydrochloride (ACB-HCl) is studied as a function of temperature and pressure by using dynamic light scattering and broadband dielectric spectroscopy. These unique experimental data provide the first direct evidence that the decoupling between the charge transport and structural relaxation exists in proton conductors over a wide T-P thermodynamic space, with the time scale of structural relaxation being constant at the liquid-glass transition (τα = 1000 s). We demonstrate that the enhanced proton transport, being a combination of intermolecular H+ hopping between cation and anion as well as tautomerization process within amide moiety of ACB molecule, results in a breakdown of the Stokes-Einstein relation at ambient and elevated pressure with the fractional exponent k being pressure dependent. The dT g /dP coefficient, stretching exponent βKWW and dynamic modulus E a /ΔV # were found to be the same regardless of the relaxation processes studied. This is in contrast to the apparent activation volume parameter that is different when charge transport and structural dynamics are considered. These experimental results together with theoretical considerations create new ideas to design efficient proton conductors for potential electrochemical applications.
format	article
author	Z. Wojnarowska M. Rams-Baron J. Knapik-Kowalczuk A. Połatyńska M. Pochylski J. Gapinski A. Patkowski P. Wlodarczyk M. Paluch
author_facet	Z. Wojnarowska M. Rams-Baron J. Knapik-Kowalczuk A. Połatyńska M. Pochylski J. Gapinski A. Patkowski P. Wlodarczyk M. Paluch
author_sort	Z. Wojnarowska
title	Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
title_short	Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
title_full	Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
title_fullStr	Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
title_full_unstemmed	Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
title_sort	experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/340efe071e10419eb5a2e39eb4d572d8
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_version_	1718385138992152576

Experimental evidence of high pressure decoupling between charge transport and structural dynamics in a protic ionic glass-former

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