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https://hdl.handle.net/2445/222727
Title: | Size-Dependent Ab Initio Atomistic Thermodynamics from Cluster to Bulk: Application to Hydration of Titania Nanoparticles |
Author: | Recio-Poo, Miguel Morales García, Ángel Illas i Riera, Francesc Bromley, Stefan Thomas |
Keywords: | Oscil·lacions Hidratació Òxids Oscillations Hydration Oxides |
Issue Date: | 6-Aug-2024 |
Publisher: | American Chemical Society |
Abstract: | 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). |
Note: | Reproducció del document publicat a: https://doi.org/10.1021/acs.jpclett.4c01531 |
It is part of: | Journal of Physical Chemistry Letters, 2024, p. 8240-8247 |
URI: | https://hdl.handle.net/2445/222727 |
Related resource: | https://doi.org/10.1021/acs.jpclett.4c01531 |
ISSN: | 1948-7185 |
Appears in Collections: | Articles publicats en revistes (Ciència dels Materials i Química Física) Articles publicats en revistes (Institut de Química Teòrica i Computacional (IQTCUB)) |
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