Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates

Tesis Doctoral inédita leída en la Universidad Autónoma de Madrid, Facultad de Ciencias, Departamento de Química. Fecha de Lectura: 19-10-2023

Detalles Bibliográficos
Autor: Yanes Rodríguez, Raquel
Tipo de recurso: tesis doctoral
Fecha de publicación:2023
País:España
Institución:Universidad Autónoma de Madrid
Repositorio:Biblos-e Archivo. Repositorio Institucional de la UAM
Idioma:inglés
OAI Identifier:oai:repositorio.uam.es:10486/712881
Acceso en línea:http://hdl.handle.net/10486/712881
Access Level:acceso abierto
Palabra clave:Gases nobles - Enlaces químicos
Van der Waals, fuerzas de
Fuerzas intermoleculares
Química
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dc.title.none.fl_str_mv Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
Estudios computacionales de propiedades termodinámicas de sistemas nanoconfinados: inclusión de He en hidratos
title Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
spellingShingle Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
Yanes Rodríguez, Raquel
Gases nobles - Enlaces químicos
Van der Waals, fuerzas de
Fuerzas intermoleculares
Química
title_short Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
title_full Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
title_fullStr Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
title_full_unstemmed Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
title_sort Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydrates
dc.creator.none.fl_str_mv Yanes Rodríguez, Raquel
author Yanes Rodríguez, Raquel
author_facet Yanes Rodríguez, Raquel
author_role author
dc.contributor.none.fl_str_mv Prosmiti, Aristea
Departamento de Química
Facultad de Ciencias
CSIC. Instituto de Física Fundamental (IFF)
dc.subject.none.fl_str_mv Gases nobles - Enlaces químicos
Van der Waals, fuerzas de
Fuerzas intermoleculares
Química
topic Gases nobles - Enlaces químicos
Van der Waals, fuerzas de
Fuerzas intermoleculares
Química
description Tesis Doctoral inédita leída en la Universidad Autónoma de Madrid, Facultad de Ciencias, Departamento de Química. Fecha de Lectura: 19-10-2023
publishDate 2023
dc.date.none.fl_str_mv 2023
2023-10-19
dc.type.none.fl_str_mv doctoral thesis
http://purl.org/coar/resource_type/c_db06
NA
http://purl.org/coar/version/c_be7fb7dd8ff6fe43
dc.type.openaire.fl_str_mv info:eu-repo/semantics/doctoralThesis
format doctoralThesis
dc.identifier.none.fl_str_mv http://hdl.handle.net/10486/712881
url http://hdl.handle.net/10486/712881
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
Attribution-NonCommercial-NoDerivatives 4.0 International
http://creativecommons.org/licenses/by-nc-nd/4.0/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv application/pdf
dc.source.none.fl_str_mv reponame:Biblos-e Archivo. Repositorio Institucional de la UAM
instname:Universidad Autónoma de Madrid
instname_str Universidad Autónoma de Madrid
reponame_str Biblos-e Archivo. Repositorio Institucional de la UAM
collection Biblos-e Archivo. Repositorio Institucional de la UAM
repository.name.fl_str_mv
repository.mail.fl_str_mv
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spelling Computational studies on thermodynamics properties of nanoconfined systems: He inclusion in hydratesEstudios computacionales de propiedades termodinámicas de sistemas nanoconfinados: inclusión de He en hidratosYanes Rodríguez, RaquelGases nobles - Enlaces químicosVan der Waals, fuerzas deFuerzas intermolecularesQuímicaTesis Doctoral inédita leída en la Universidad Autónoma de Madrid, Facultad de Ciencias, Departamento de Química. Fecha de Lectura: 19-10-2023Esta tesis tiene embargado el acceso al texto completo hasta el 19-04-2025The primary focus of this thesis is to study the impact of incorporating helium atoms into hydrostructures, spanning from clathrate-like and ice-like clusters up to complete periodic crystalline systems. Noble-gas hydrates are of particular interest, due to their ability to keep trapped such inert gases. The recent synthesis of some noble gas (Ne, He) clathrate hydrates and the previously reported presence of He in ice frameworks, as well as their potential implication in the stabilization and discovery of new low-density ices, combined with the limited information available on such hydrates, serve as strong motivations to expand our understanding of these relatively unexplored systems. One of the main features of these He-filled structures is the stability conferred by the weak van der Waals dispersion forces occurred between the host lattice and the guest atoms (noble gas in our case), in addition to the hydrogen bonds established among the water molecules. Hence, it is crucial to have reliable reference data in order to accurately describe these interactions. As a result, the first part of this thesis is devoted to the systematic examination of the performance and accuracy of various conventional and modern DFT functionals, as well as available analytical model potentials, in comparison with high-level, well-converged wave function-based datasets. In this manner, benchmark reference datasets for He@hydrate frameworks are gathered and utilized to identify the computationally viable, best-performing DFT functionals. Minimum and non-minimun configurations of a selection of clathrate-like and ice-like fundamental units and building blocks are considered in order to ensure a correct characterization of the underlying forces in repulsive, near-equilibrium, and asymptotic/long-range regions of the full potential energy surface. As the quality of the data has profound implications on the development of models, the outcome of such benchmark studies becomes essential guidance for forthcoming new chem-informatics potentials and force-fields models. Enthalpy, Gibbs free energy and entropy are practical and important thermodynamic properties, that provide valuable information about the course of a formation/dissociation reaction. The second part of this thesis involves utilizing first-principles DFT approaches to analyse the variations in H, G, and S under different T-P conditions, specifically focusing on the encapsulation of He atoms within sII clathrate-like cages, both individual or connected to their neighbor cage, and ice II/ice XVII individual channels. Moreover, we investigate the feasibility of including an increased number of He atoms inside the different size cages of the sII structure, assessing structural and energetic properties such as binding or evaporation energies. The idea of this investigation is to determine whether it is viable to obtain a meaningful and orientative initial estimate regarding the thermodynamic feasibility and spontaneous nature of the formation process of He-filled clathrate/ice structures through the analysis of finite-size clathrate-like and ice-like cluster frameworksLa realización de esta tesis ha sido posible gracias a la financiación brindada por los proyectos FIS2017- 83157-P (MINECO), IND2018/TIC-9467 (COMUNIDAD DE MADRID) y PID2020-114654GB-I00 (MICINN), así como COST Actions CA18212(MDGAS) y CA21101(COSY)Prosmiti, AristeaDepartamento de QuímicaFacultad de CienciasCSIC. Instituto de Física Fundamental (IFF)20232023-10-19doctoral thesishttp://purl.org/coar/resource_type/c_db06NAhttp://purl.org/coar/version/c_be7fb7dd8ff6fe43info:eu-repo/semantics/doctoralThesisapplication/pdfhttp://hdl.handle.net/10486/712881reponame:Biblos-e Archivo. Repositorio Institucional de la UAMinstname:Universidad Autónoma de MadridInglésengopen accesshttp://purl.org/coar/access_right/c_abf2Attribution-NonCommercial-NoDerivatives 4.0 Internationalhttp://creativecommons.org/licenses/by-nc-nd/4.0/info:eu-repo/semantics/openAccessoai:repositorio.uam.es:10486/7128812026-06-23T12:46:27Z
score 15,81155

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