Articles producció científica> Química Física i Inorgànica

Data-driven models for ground and excited states for Single Atoms on Ceria

  • Identification data

    Identifier: imarina:9280702
    Authors:
    Geiger, JulianSabadell-Rendon, AlbertDaelman, NathanLopez, Nuria
    Abstract:
    Ceria-based single-atom catalysts present complex electronic structures due to the dynamic electron transfer between the metal atoms and the semiconductor oxide support. Understanding these materials implies retrieving all states in these electronic ensembles, which can be limiting if done via density functional theory. Here, we propose a data-driven approach to obtain a parsimonious model identifying the appearance of dynamic charge transfer for the single atoms (SAs). We first constructed a database of (701) electronic configurations for the group 9-11 metals on CeO2(100). Feature Selection based on predictive Elastic Net and Random Forest models highlights eight fundamental variables: atomic number, ionization potential, size, and metal coordination, metal-oxygen bond strengths, surface strain, and Coulomb interactions. With these variables a Bayesian algorithm yields an expression for the adsorption energies of SAs in ground and low-lying excited states. Our work paves the way towards understanding electronic structure complexity in metal/oxide interfaces.
  • Others:

    Author, as appears in the article.: Geiger, Julian; Sabadell-Rendon, Albert; Daelman, Nathan; Lopez, Nuria;
    Department: Química Física i Inorgànica
    URV's Author/s: Geiger, Julian / Lopez Alonso, Nuria / Sabadell Rendón, Albert
    Keywords: Oxide Oxidation Computational chemistry Co Catalysis
    Abstract: Ceria-based single-atom catalysts present complex electronic structures due to the dynamic electron transfer between the metal atoms and the semiconductor oxide support. Understanding these materials implies retrieving all states in these electronic ensembles, which can be limiting if done via density functional theory. Here, we propose a data-driven approach to obtain a parsimonious model identifying the appearance of dynamic charge transfer for the single atoms (SAs). We first constructed a database of (701) electronic configurations for the group 9-11 metals on CeO2(100). Feature Selection based on predictive Elastic Net and Random Forest models highlights eight fundamental variables: atomic number, ionization potential, size, and metal coordination, metal-oxygen bond strengths, surface strain, and Coulomb interactions. With these variables a Bayesian algorithm yields an expression for the adsorption energies of SAs in ground and low-lying excited states. Our work paves the way towards understanding electronic structure complexity in metal/oxide interfaces.
    Thematic Areas: Modeling and simulation Mechanics of materials Materials science, multidisciplinary Materials science (miscellaneous) Materials science (all) General materials science Computer science applications Chemistry, physical
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    Author's mail: nuria.lopez@urv.cat julian.geiger@estudiants.urv.cat albert.sabadell@estudiants.urv.cat
    Author identifier: 0000-0003-0023-1960
    Record's date: 2024-09-07
    Papper version: info:eu-repo/semantics/publishedVersion
    Link to the original source: https://www.nature.com/articles/s41524-022-00852-1
    Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
    Papper original source: Npj Computational Materials. 8 (1):
    APA: Geiger, Julian; Sabadell-Rendon, Albert; Daelman, Nathan; Lopez, Nuria; (2022). Data-driven models for ground and excited states for Single Atoms on Ceria. Npj Computational Materials, 8(1), -. DOI: 10.1038/s41524-022-00852-1
    Article's DOI: 10.1038/s41524-022-00852-1
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2022
    Publication Type: Journal Publications
  • Keywords:

    Chemistry, Physical,Computer Science Applications,Materials Science (Miscellaneous),Materials Science, Multidisciplinary,Mechanics of Materials,Modeling and Simulation
    Oxide
    Oxidation
    Computational chemistry
    Co
    Catalysis
    Modeling and simulation
    Mechanics of materials
    Materials science, multidisciplinary
    Materials science (miscellaneous)
    Materials science (all)
    General materials science
    Computer science applications
    Chemistry, physical
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