Articles producció científica> Química Física i Inorgànica

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

  • Dades identificatives

    Identificador: imarina:9280702
    Autors:
    Geiger, JulianSabadell-Rendon, AlbertDaelman, NathanLopez, Nuria
    Resum:
    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.
  • Altres:

    Autor segons l'article: Geiger, Julian; Sabadell-Rendon, Albert; Daelman, Nathan; Lopez, Nuria;
    Departament: Química Física i Inorgànica
    Autor/s de la URV: Geiger, Julian / Lopez Alonso, Nuria / Sabadell Rendón, Albert
    Paraules clau: Oxide Oxidation Computational chemistry Co Catalysis
    Resum: 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.
    Àrees temàtiques: Modeling and simulation Mechanics of materials Materials science, multidisciplinary Materials science (miscellaneous) Materials science (all) General materials science Computer science applications Chemistry, physical
    Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
    Adreça de correu electrònic de l'autor: nuria.lopez@urv.cat julian.geiger@estudiants.urv.cat albert.sabadell@estudiants.urv.cat
    Identificador de l'autor: 0000-0003-0023-1960
    Data d'alta del registre: 2024-09-07
    Versió de l'article dipositat: info:eu-repo/semantics/publishedVersion
    Enllaç font original: https://www.nature.com/articles/s41524-022-00852-1
    URL Document de llicència: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referència a l'article segons font original: Npj Computational Materials. 8 (1):
    Referència de l'ítem segons les normes 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
    DOI de l'article: 10.1038/s41524-022-00852-1
    Entitat: Universitat Rovira i Virgili
    Any de publicació de la revista: 2022
    Tipus de publicació: Journal Publications
  • Paraules clau:

    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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