Articles producció científica> Química Física i Inorgànica

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

  • Identification data

    Identifier: imarina:9282008
    Authors:
    Giulimondi VRuiz–Ferrando AClark AHKaiser SKKrumeich FMartín AJLópez NPérez–Ramírez J
    Abstract:
    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.
  • Others:

    Author, as appears in the article.: Giulimondi V; Ruiz–Ferrando A; Clark AH; Kaiser SK; Krumeich F; Martín AJ; López N; Pérez–Ramírez J
    Department: Química Física i Inorgànica
    URV's Author/s: Lopez Alonso, Nuria / Ruiz Ferrando, Andrea
    Keywords: Total-energy calculations Single–atom catalysts Single-atom catalysts Mechanism Hydrogen evolution reaction Gold Cooperativity effects Chemistry Carbon Bimetallic systems Active site coordination
    Abstract: 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.
    Thematic Areas: 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
    licence for use: https://creativecommons.org/licenses/by/3.0/es/
    Author's mail: nuria.lopez@urv.cat andrea.ruizf@estudiants.urv.cat
    Record's date: 2024-09-07
    Papper version: info:eu-repo/semantics/publishedVersion
    Link to the original source: https://onlinelibrary.wiley.com/doi/full/10.1002/adfm.202206513
    Licence document URL: https://repositori.urv.cat/ca/proteccio-de-dades/
    Papper original source: Advanced Functional Materials.
    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
    Article's DOI: 10.1002/adfm.202206513
    Entity: Universitat Rovira i Virgili
    Journal publication year: 2022
    Publication Type: Journal Publications
  • Keywords:

    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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