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