Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles

Ab initio atomistic thermodynamics (AIAT) has become an indispensable tool to estimate Gibbs free energy changes for solid surfaces interacting with gaseous species relative to pressure (p) and temperature (T). For such systems, AIAT assumes that solid vibrational contributions to Gibbs free energy...

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Autores: Recio-Poo, Miguel, Morales García, Ángel, Illas i Riera, Francesc, Bromley, Stefan Thomas
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/222727
Acceso en línea:https://hdl.handle.net/2445/222727
Access Level:acceso abierto
Palabra clave:Oscil·lacions
Hidratació
Òxids
Oscillations
Hydration
Oxides
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spelling Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania NanoparticlesRecio-Poo, MiguelMorales García, ÁngelIllas i Riera, FrancescBromley, Stefan ThomasOscil·lacionsHidratacióÒxidsOscillationsHydrationOxidesAb initio atomistic thermodynamics (AIAT) has become an indispensable tool to estimate Gibbs free energy changes for solid surfaces interacting with gaseous species relative to pressure (p) and temperature (T). For such systems, AIAT assumes that solid vibrational contributions to Gibbs free energy differences cancel out. However, the validity of this assumption is unclear for nanoscale systems. Using hydrated titania nanoparticles (NPs) as an example, we estimate the vibrational contributions to the Gibbs free energy of hydration (ΔGhyd(T,p)) for arbitrary NP size and degree of hydration. Comparing ΔGhyd(T,p) phase diagrams for NPs when considering these contributions (AIATnano) relative to a standard AIAT approach reveals significant qualitative and quantitative differences, which only become negligible for large systems. By constructing a size-dependent ΔGhyd(T,p) phase diagram, we illustrate how our approach can provide deeper insights into how nanosytems interact with their environments, with many potential applications (e.g., catalytic nanoparticles, biological colloids, nanoparticulate pollutants).American Chemical Society2025202520242025info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersion8 p.application/pdfhttps://hdl.handle.net/2445/222727Articles publicats en revistes (Ciència dels Materials i Química Física)reponame:Recercat. Dipósit de la Recerca de Catalunyainstname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)InglésReproducció del document publicat a: https://doi.org/10.1021/acs.jpclett.4c01531Journal of Physical Chemistry Letters, 2024, p. 8240-8247https://doi.org/10.1021/acs.jpclett.4c01531cc-by (c) Recio-Poo, Miguel, et al., 2024http://creativecommons.org/licenses/by/3.0/es/info:eu-repo/semantics/openAccessoai:recercat.cat:2445/2227272026-05-29T05:05:01Z
dc.title.none.fl_str_mv Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
title Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
spellingShingle Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
Recio-Poo, Miguel
Oscil·lacions
Hidratació
Òxids
Oscillations
Hydration
Oxides
title_short Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
title_full Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
title_fullStr Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
title_full_unstemmed Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
title_sort Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles
dc.creator.none.fl_str_mv Recio-Poo, Miguel
Morales García, Ángel
Illas i Riera, Francesc
Bromley, Stefan Thomas
author Recio-Poo, Miguel
author_facet Recio-Poo, Miguel
Morales García, Ángel
Illas i Riera, Francesc
Bromley, Stefan Thomas
author_role author
author2 Morales García, Ángel
Illas i Riera, Francesc
Bromley, Stefan Thomas
author2_role author
author
author
dc.subject.none.fl_str_mv Oscil·lacions
Hidratació
Òxids
Oscillations
Hydration
Oxides
topic Oscil·lacions
Hidratació
Òxids
Oscillations
Hydration
Oxides
description Ab initio atomistic thermodynamics (AIAT) has become an indispensable tool to estimate Gibbs free energy changes for solid surfaces interacting with gaseous species relative to pressure (p) and temperature (T). For such systems, AIAT assumes that solid vibrational contributions to Gibbs free energy differences cancel out. However, the validity of this assumption is unclear for nanoscale systems. Using hydrated titania nanoparticles (NPs) as an example, we estimate the vibrational contributions to the Gibbs free energy of hydration (ΔGhyd(T,p)) for arbitrary NP size and degree of hydration. Comparing ΔGhyd(T,p) phase diagrams for NPs when considering these contributions (AIATnano) relative to a standard AIAT approach reveals significant qualitative and quantitative differences, which only become negligible for large systems. By constructing a size-dependent ΔGhyd(T,p) phase diagram, we illustrate how our approach can provide deeper insights into how nanosytems interact with their environments, with many potential applications (e.g., catalytic nanoparticles, biological colloids, nanoparticulate pollutants).
publishDate 2024
dc.date.none.fl_str_mv 2024
2025
2025
2025
dc.type.none.fl_str_mv info:eu-repo/semantics/article
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv https://hdl.handle.net/2445/222727
url https://hdl.handle.net/2445/222727
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv Reproducció del document publicat a: https://doi.org/10.1021/acs.jpclett.4c01531
Journal of Physical Chemistry Letters, 2024, p. 8240-8247
https://doi.org/10.1021/acs.jpclett.4c01531
dc.rights.none.fl_str_mv cc-by (c) Recio-Poo, Miguel, et al., 2024
http://creativecommons.org/licenses/by/3.0/es/
info:eu-repo/semantics/openAccess
rights_invalid_str_mv cc-by (c) Recio-Poo, Miguel, et al., 2024
http://creativecommons.org/licenses/by/3.0/es/
eu_rights_str_mv openAccess
dc.format.none.fl_str_mv 8 p.
application/pdf
dc.publisher.none.fl_str_mv American Chemical Society
publisher.none.fl_str_mv American Chemical Society
dc.source.none.fl_str_mv Articles publicats en revistes (Ciència dels Materials i Química Física)
reponame:Recercat. Dipósit de la Recerca de Catalunya
instname:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
instname_str Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
reponame_str Recercat. Dipósit de la Recerca de Catalunya
collection Recercat. Dipósit de la Recerca de Catalunya
repository.name.fl_str_mv
repository.mail.fl_str_mv
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score 15.812455

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