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Ab initio molecular dynamics study of metal oxide-water interfaces and development of polarizable force field
Stockholm University, Faculty of Science, Department of Chemistry.
2025 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

This thesis describes a computational study of interfaces between water and metal oxides using classical and ab initio molecular dynamics simulations. Specifically, the work focuses on different surfaces of the metal oxides TiO2 and ZnO. A number of different systems were simulated including ideal flat surfaces, a curved nanoparticle surface as well as surfaces with oxygen vacancies. It was investigated how the properties of water change near the metal oxide - water interface and what reactions water molecules undergo in these systems. Furthermore, classical force fields describing interactions in TiO2, ZnO and their hydrated surfaces were developed. This was done by partitioning of electron density from ab initio molecular dynamics simulations combined with scaling theories relating atomic volumes to polarizabilities and dispersion coefficients. For TiO2 a polarizable force field based on the Drude oscillator model was developed. The results give new atomistic insight into water structure, dynamics and reactivity on metal oxide surfaces and highlights the importance of polarizability for accurate modeling of water adsorption thermodynamics.

Place, publisher, year, edition, pages
Stockholm: Department of Chemistry, Stockholm University , 2025. , p. 80
Keywords [en]
Nanomaterials, Metal oxide - water interfaces, Molecular dynamics simulations
National Category
Physical Chemistry
Research subject
Physical Chemistry
Identifiers
URN: urn:nbn:se:su:diva-237495ISBN: 978-91-8107-072-9 (print)ISBN: 978-91-8107-073-6 (electronic)OAI: oai:DiVA.org:su-237495DiVA, id: diva2:1924263
Public defence
2025-02-21, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 14:00 (English)
Opponent
Supervisors
Available from: 2025-01-29 Created: 2025-01-03 Last updated: 2025-01-29Bibliographically approved
List of papers
1. Water structure, dynamics and reactivity on a TiO2-nanoparticle surface: new insights from ab initio molecular dynamics
Open this publication in new window or tab >>Water structure, dynamics and reactivity on a TiO2-nanoparticle surface: new insights from ab initio molecular dynamics
2022 (English)In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 14, no 44, p. 16536-16547Article in journal (Refereed) Published
National Category
Natural Sciences
Identifiers
urn:nbn:se:su:diva-237480 (URN)10.1039/d2nr02354g (DOI)
Funder
EU, Horizon 2020, NanoSolveIt projectSwedish Research Council, 2021-04474
Available from: 2025-01-02 Created: 2025-01-02 Last updated: 2025-01-03
2. Oxygen vacancies on hydrated anatase (101) surfaces: Insights from classical and ab initio molecular dynamics simulations
Open this publication in new window or tab >>Oxygen vacancies on hydrated anatase (101) surfaces: Insights from classical and ab initio molecular dynamics simulations
(English)Manuscript (preprint) (Other academic)
National Category
Natural Sciences
Identifiers
urn:nbn:se:su:diva-237488 (URN)
Available from: 2025-01-02 Created: 2025-01-02 Last updated: 2025-01-10
3. Ab Initio Derived Classical Force Field for Molecular Dynamics Simulations of ZnO Surfaces in Biological Environment
Open this publication in new window or tab >>Ab Initio Derived Classical Force Field for Molecular Dynamics Simulations of ZnO Surfaces in Biological Environment
2023 (English)In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 127, no 25, p. 5446-5457Article in journal (Refereed) Published
Abstract [en]

Zinc oxide nanostructures are used in an ever increasing line of applications in technology and biomedical fields. This requires a detailed understanding of the phenomena that occur at the surface particularly in aqueous environments and in contact with biomolecules. In this work, we used ab initio molecular dynamics (AIMD) simulations to determine structural details of ZnO surfaces in water and to develop a general and transferable classical force field for hydrated ZnO surfaces. AIMD simulations show that water molecules dissociate near unmodified ZnO surfaces, forming hydroxyl groups at about 65% of the surface Zn atoms and protonating 3-coordinated surface oxygen atoms, while the rest of the surface Zn atoms bind molecularly adsorbed waters. Several force field atom types for ZnO surface atoms were identified by analysis of the specific connectivities of atoms. The analysis of the electron density was then used to determine partial charges and Lennard-Jones parameters for the identified force field atom types. The obtained force field was validated by comparison with AIMD results and with available experimental data on adsorption and immersion enthalpies, as well as adsorption free energies of several amino acids in methanol. The developed force field can be used for modeling of ZnO in aqueous and other fluid environments and in interaction with biomolecules.

National Category
Physical Chemistry
Identifiers
urn:nbn:se:su:diva-229531 (URN)10.1021/acs.jpca.3c00424 (DOI)001009945900001 ()37314246 (PubMedID)2-s2.0-85163509873 (Scopus ID)
Available from: 2024-05-24 Created: 2024-05-24 Last updated: 2025-01-03Bibliographically approved
4. Polarizable force field for TiO2 based on the Drude oscillator model
Open this publication in new window or tab >>Polarizable force field for TiO2 based on the Drude oscillator model
2024 (English)In: AIP Advances, E-ISSN 2158-3226, Vol. 14, no 11Article in journal (Refereed) Published
National Category
Natural Sciences
Identifiers
urn:nbn:se:su:diva-237485 (URN)10.1063/5.0242166 (DOI)
Funder
Swedish Research Council, 2021-04474
Available from: 2025-01-02 Created: 2025-01-02 Last updated: 2025-01-03

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Grote, Fredrik

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  • de-DE
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Output format
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