Articles producció científica> Química Física i Inorgànica

Catalytic Synergies in Bimetallic Ru-Pt Single-Atom Catalysts via Speciation Control

  • Datos identificativos

    Identificador: imarina:9282008
    Autores:
    Giulimondi VRuiz–Ferrando AClark AHKaiser SKKrumeich FMartín AJLópez NPérez–Ramírez J
    Resumen:
    Bimetallic single-atom catalysts (b-SACs) have recently gained prominence by virtue of the unique catalytic cooperative interactions they can exhibit, intertwining electronic and geometric effects. To date, research efforts have exclusively focused on direct mechanisms such as electron density transfer or sequential reactivity. Herein, the first study on indirect, coordination-induced catalytic synergies in carbon-supported Ru-Pt SACs is conducted. To this end, a holistic approach is developed, combining i) precision synthesis, ii) advanced characterization, iii) exploration of single-site adsorption properties via the hydrogen evolution reaction, and iv) modeling through density functional theory. Despite the lack of both intermetallic coordination in the first or second shell and charge redistribution effects, the Ru-Pt SACs exhibit a H-2 formation rate enhanced up to 15-fold compared with their monometallic counterparts. To unfold the origin of the intermetallic cooperativity, modifications of the structural and catalytic properties induced by the integration of a second metal species are investigated. Thus, Pt atoms are found to selectively occupy the most energeticallyfavorable cavities in the support, prompting Ru atoms to assume a distinct, more active, configuration. This contribution unveils a novel principle of bimetallic cooperativity, demonstrating the key role of integrative experimental and computational analyses in studying b-SACs.
  • Otros:

    Autor según el artículo: Giulimondi V; Ruiz–Ferrando A; Clark AH; Kaiser SK; Krumeich F; Martín AJ; López N; Pérez–Ramírez J
    Departamento: Química Física i Inorgànica
    Autor/es de la URV: Lopez Alonso, Nuria / Ruiz Ferrando, Andrea
    Palabras clave: Total-energy calculations Single–atom catalysts Single-atom catalysts Mechanism Hydrogen evolution reaction Gold Cooperativity effects Chemistry Carbon Bimetallic systems Active site coordination
    Resumen: Bimetallic single-atom catalysts (b-SACs) have recently gained prominence by virtue of the unique catalytic cooperative interactions they can exhibit, intertwining electronic and geometric effects. To date, research efforts have exclusively focused on direct mechanisms such as electron density transfer or sequential reactivity. Herein, the first study on indirect, coordination-induced catalytic synergies in carbon-supported Ru-Pt SACs is conducted. To this end, a holistic approach is developed, combining i) precision synthesis, ii) advanced characterization, iii) exploration of single-site adsorption properties via the hydrogen evolution reaction, and iv) modeling through density functional theory. Despite the lack of both intermetallic coordination in the first or second shell and charge redistribution effects, the Ru-Pt SACs exhibit a H-2 formation rate enhanced up to 15-fold compared with their monometallic counterparts. To unfold the origin of the intermetallic cooperativity, modifications of the structural and catalytic properties induced by the integration of a second metal species are investigated. Thus, Pt atoms are found to selectively occupy the most energeticallyfavorable cavities in the support, prompting Ru atoms to assume a distinct, more active, configuration. This contribution unveils a novel principle of bimetallic cooperativity, demonstrating the key role of integrative experimental and computational analyses in studying b-SACs.
    Áreas temáticas: Química Physics, condensed matter Physics, applied Nanoscience and nanotechnology Nanoscience & nanotechnology Materials science, multidisciplinary Materials science (miscellaneous) Materials science (all) Materiais General materials science General chemistry Engenharias iv Engenharias ii Electronic, optical and magnetic materials Electrochemistry Condensed matter physics Ciências agrárias i Chemistry, physical Chemistry, multidisciplinary Chemistry (miscellaneous) Chemistry (all) Biomaterials Astronomia / física
    Acceso a la licencia de uso: https://creativecommons.org/licenses/by/3.0/es/
    Direcció de correo del autor: nuria.lopez@urv.cat andrea.ruizf@estudiants.urv.cat
    Fecha de alta del registro: 2024-09-07
    Versión del articulo depositado: info:eu-repo/semantics/publishedVersion
    Enlace a la fuente original: https://onlinelibrary.wiley.com/doi/full/10.1002/adfm.202206513
    URL Documento de licencia: https://repositori.urv.cat/ca/proteccio-de-dades/
    Referencia al articulo segun fuente origial: Advanced Functional Materials.
    Referencia de l'ítem segons les normes APA: Giulimondi V; Ruiz–Ferrando A; Clark AH; Kaiser SK; Krumeich F; Martín AJ; López N; Pérez–Ramírez J (2022). Catalytic Synergies in Bimetallic Ru-Pt Single-Atom Catalysts via Speciation Control. Advanced Functional Materials, (), -. DOI: 10.1002/adfm.202206513
    DOI del artículo: 10.1002/adfm.202206513
    Entidad: Universitat Rovira i Virgili
    Año de publicación de la revista: 2022
    Tipo de publicación: Journal Publications
  • Palabras clave:

    Biomaterials,Chemistry (Miscellaneous),Chemistry, Multidisciplinary,Chemistry, Physical,Condensed Matter Physics,Electrochemistry,Electronic, Optical and Magnetic Materials,Materials Science (Miscellaneous),Materials Science, Multidisciplinary,Nanoscience & Nanotechnology,Nanoscience and Nanotechnology,Physics, Applied,Physics, Condensed M
    Total-energy calculations
    Single–atom catalysts
    Single-atom catalysts
    Mechanism
    Hydrogen evolution reaction
    Gold
    Cooperativity effects
    Chemistry
    Carbon
    Bimetallic systems
    Active site coordination
    Química
    Physics, condensed matter
    Physics, applied
    Nanoscience and nanotechnology
    Nanoscience & nanotechnology
    Materials science, multidisciplinary
    Materials science (miscellaneous)
    Materials science (all)
    Materiais
    General materials science
    General chemistry
    Engenharias iv
    Engenharias ii
    Electronic, optical and magnetic materials
    Electrochemistry
    Condensed matter physics
    Ciências agrárias i
    Chemistry, physical
    Chemistry, multidisciplinary
    Chemistry (miscellaneous)
    Chemistry (all)
    Biomaterials
    Astronomia / física
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