Autor segons l'article: Giulimondi V; Ruiz–Ferrando A; Clark AH; Kaiser SK; Krumeich F; Martín AJ; López N; Pérez–Ramírez J
Departament: Química Física i Inorgànica
Autor/s de la URV: Lopez Alonso, Nuria / Ruiz Ferrando, Andrea
Paraules clau: Active site coordination Bimetallic systems Carbon Chemistry Cooperativity effects Gold Hydrogen evolution reaction Mechanism Single-atom catalysts Single–atom catalysts Total-energy calculations
Resum: 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.
Àrees temàtiques: Astronomia / física Biomaterials Chemistry (all) Chemistry (miscellaneous) Chemistry, multidisciplinary Chemistry, physical Ciências agrárias i Condensed matter physics Electrochemistry Electronic, optical and magnetic materials Engenharias ii Engenharias iv General chemistry General materials science Materiais Materials science (all) Materials science (miscellaneous) Materials science, multidisciplinary Nanoscience & nanotechnology Nanoscience and nanotechnology Physics, applied Physics, condensed matter Química
Accès a la llicència d'ús: https://creativecommons.org/licenses/by/3.0/es/
Adreça de correu electrònic de l'autor: andrea.ruizf@estudiants.urv.cat nuria.lopez@urv.cat
Data d'alta del registre: 2024-01-13
Versió de l'article dipositat: info:eu-repo/semantics/publishedVersion
Enllaç font original: https://onlinelibrary.wiley.com/doi/full/10.1002/adfm.202206513
Referència a l'article segons font original: Advanced Functional Materials.
Referència 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
URL Document de llicència: http://repositori.urv.cat/ca/proteccio-de-dades/
DOI de l'article: 10.1002/adfm.202206513
Entitat: Universitat Rovira i Virgili
Any de publicació de la revista: 2022
Tipus de publicació: Journal Publications
Repositori URV