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Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure

Studies of the structure of hydroxides under pressure using neutron diffraction reveal that the high concentration of hydrogen is distributed in a disordered network. The disorder in the hydrogen-bond network and possible phase transitions are reported to occur at pressures within the range accessib...

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Autores principales: Dupuis, Romain, Dolado, Jorge S., Benoit, Magali, Surga, Jose, Ayuela, Andrés
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5501843/
https://www.ncbi.nlm.nih.gov/pubmed/28687787
http://dx.doi.org/10.1038/s41598-017-04080-2
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author Dupuis, Romain
Dolado, Jorge S.
Benoit, Magali
Surga, Jose
Ayuela, Andrés
author_facet Dupuis, Romain
Dolado, Jorge S.
Benoit, Magali
Surga, Jose
Ayuela, Andrés
author_sort Dupuis, Romain
collection PubMed
description Studies of the structure of hydroxides under pressure using neutron diffraction reveal that the high concentration of hydrogen is distributed in a disordered network. The disorder in the hydrogen-bond network and possible phase transitions are reported to occur at pressures within the range accessible to experiments for layered calcium hydroxides, which are considered to be exemplary prototype materials. In this study, the static and dynamical properties of these layered hydroxides are investigated using a quantum approach describing nuclear motion, shown herein to be required particularly when studying diffusion processes involving light hydrogen atoms. The effect of high-pressure on the disordered hydrogen-bond network shows that the protons tunnel back and forth across the barriers between three potential minima around the oxygen atoms. At higher pressures the structure has quasi two-dimensional layers of hydrogen atoms, such that at low temperatures this causes the barrier crossing of the hydrogen to be significantly rarefied. Furthermore, for moderate values of both temperature and pressure this process occurs less often than the usual mechanism of proton transport via vacancies, limiting global proton diffusion within layers at high pressure.
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spelling pubmed-55018432017-07-10 Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure Dupuis, Romain Dolado, Jorge S. Benoit, Magali Surga, Jose Ayuela, Andrés Sci Rep Article Studies of the structure of hydroxides under pressure using neutron diffraction reveal that the high concentration of hydrogen is distributed in a disordered network. The disorder in the hydrogen-bond network and possible phase transitions are reported to occur at pressures within the range accessible to experiments for layered calcium hydroxides, which are considered to be exemplary prototype materials. In this study, the static and dynamical properties of these layered hydroxides are investigated using a quantum approach describing nuclear motion, shown herein to be required particularly when studying diffusion processes involving light hydrogen atoms. The effect of high-pressure on the disordered hydrogen-bond network shows that the protons tunnel back and forth across the barriers between three potential minima around the oxygen atoms. At higher pressures the structure has quasi two-dimensional layers of hydrogen atoms, such that at low temperatures this causes the barrier crossing of the hydrogen to be significantly rarefied. Furthermore, for moderate values of both temperature and pressure this process occurs less often than the usual mechanism of proton transport via vacancies, limiting global proton diffusion within layers at high pressure. Nature Publishing Group UK 2017-07-07 /pmc/articles/PMC5501843/ /pubmed/28687787 http://dx.doi.org/10.1038/s41598-017-04080-2 Text en © The Author(s) 2017 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Dupuis, Romain
Dolado, Jorge S.
Benoit, Magali
Surga, Jose
Ayuela, Andrés
Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure
title Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure
title_full Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure
title_fullStr Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure
title_full_unstemmed Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure
title_short Quantum Nuclear Dynamics of Protons within Layered Hydroxides at High Pressure
title_sort quantum nuclear dynamics of protons within layered hydroxides at high pressure
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5501843/
https://www.ncbi.nlm.nih.gov/pubmed/28687787
http://dx.doi.org/10.1038/s41598-017-04080-2
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