CuGaO2 delafossite as a high-surface area model catalyst for Cu+-activated reactions

Copper is one of the goldilocks metals in catalysis. Deciphering the local atomic environment and oxidation state of active centers in supported copper catalysts, as well as the design of materials to control their stability under reaction conditions remains a great challenge today. We show here tha...

Descripción completa

Detalles Bibliográficos
Autores: Fornero, E.L., Murgida, G.E., Bosco, M.V., Hernández Garrido, J.C., Aguirre, A., Calaza, F.C., Stacchiola, D., Ganduglia-Pirovano, M. V., Bonivardi, A.L.
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2023
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:dnet:digitalcsic_::c00ef42abfeb44a862aed23c73afd66d
Acceso en línea:http://hdl.handle.net/10261/358235
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85171744684&doi=10.1016%2fj.jcat.2023.115107&partnerID=40&md5=cab4af4fb50e7756c25cc617dfa1acc1
Access Level:acceso abierto
Palabra clave:CO oxidation
Density functional calculations
Electron microscopy
Photoelectron spectroscopy
Time-resolved IR spectroscopy
Descripción
Sumario:Copper is one of the goldilocks metals in catalysis. Deciphering the local atomic environment and oxidation state of active centers in supported copper catalysts, as well as the design of materials to control their stability under reaction conditions remains a great challenge today. We show here that a mixed-oxide of copper delafossite with gallium (CuGaO2, Cu1+ and Ga3+) in the form of porous nanoplates, mainly exposing (1 1 0) facets with Cu1+ and Ga3+ cations in well-defined surface positions is a promising material as a model catalyst to explore the activity and stability of Cu1+-activated reactions. It is shown that the delafossite structure is preserved after calcination or reduction pretreatments (in pure O2 or H2, respectively). Extensive reduction of the mixed-oxide leads to a stable catalyst with higher activity for CO oxidation, as a result of the formation of geminal dicarbonyl species on Cuδ+, with 0 < δ < 1, under reaction conditions. © 2023