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