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dc.contributor.author
Soria, Federico Ariel
dc.contributor.author
Di Valentin, Cristiana
dc.date.available
2022-10-13T13:05:56Z
dc.date.issued
2021-02
dc.identifier.citation
Soria, Federico Ariel; Di Valentin, Cristiana; Reactive molecular dynamics simulations of hydration shells surrounding spherical TiO 2 nanoparticles: Implications for proton-transfer reactions; Royal Society of Chemistry; Nanoscale; 13; 7; 2-2021; 4151-4166
dc.identifier.issn
2040-3364
dc.identifier.uri
http://hdl.handle.net/11336/172912
dc.description.abstract
In many potential applications, nanoparticles are typically in an aqueous medium. This has strong influence on the stability, optical properties and reactivity, in particular for their functionalization. Therefore, the understanding of the chemistry at the interface between the solvent and the nanoparticle is of utmost importance. In this work, we present a comparative ReaxFF reactive molecular dynamics investigation on spherical TiO2 nanoparticles (NSs) of realistic size, with diameters from 2.2 to 4.4 nm, immersed in a large drop of bulk water. After force field validation for its use for a curved anatase TiO2 surface/water interface, we performed several simulations of the TiO2 nanoparticles of increasing size in a water drop. We found that water can be adsorbed jointly in a molecular and dissociative way on the surface. A Langmuir isotherm indicating an adsorption/desorption mechanism of water on the NS is observed. Regarding the dissociative adsorption, atomistic details reveal two different mechanisms, depending on the water concentration around the NS. At low coverage, the first mechanism involves direct dissociation of a single water molecule, whereas, at higher water coverage, the second mechanism is a proton transfer reaction involving two water molecules, also known as Grotthuss-like mechanism. Thermal annealing simulations show that several water molecules remain on the surface in agreement with the experimental reports. The capacity of adsorption is higher for the 2.2 and 3.0 nm NSs than for the 4.4 nm NS. Finally, a comparative investigation with flat surfaces indicates that NSs present a higher water adsorption capacity (undissociated and dissociated) than flat surfaces, which can be rationalized considering that NSs present many more low-coordinated Ti atoms available for water adsorption. This journal is.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
Royal Society of Chemistry
dc.rights
info:eu-repo/semantics/openAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc/2.5/ar/
dc.subject
TiO2
dc.subject
WATER
dc.subject
REAXFF
dc.subject
REACTIVITY
dc.subject.classification
Físico-Química, Ciencia de los Polímeros, Electroquímica
dc.subject.classification
Ciencias Químicas
dc.subject.classification
CIENCIAS NATURALES Y EXACTAS
dc.title
Reactive molecular dynamics simulations of hydration shells surrounding spherical TiO 2 nanoparticles: Implications for proton-transfer reactions
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2022-09-21T23:35:30Z
dc.identifier.eissn
2040-3372
dc.journal.volume
13
dc.journal.number
7
dc.journal.pagination
4151-4166
dc.journal.pais
Reino Unido
dc.journal.ciudad
Cambridge
dc.description.fil
Fil: Soria, Federico Ariel. Universita Di Milano Bicocca; Italia. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina
dc.description.fil
Fil: Di Valentin, Cristiana. Università Di Milano Bicocca; Italia
dc.journal.title
Nanoscale
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2021/NR/D0NR07503E
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/http://dx.doi.org/10.1039/D0NR07503E
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