Utilizad este identificador para citar o enlazar este documento: http://hdl.handle.net/2072/450542

Título:	Activation of Copper Species on Carbon Nitride for Enhanced Activity in the Arylation of Amines
Autor/a:	Vorobyeva, Evgeniya; Gerken, Viktoria C.; Mitchell, Sharon; Sabadell-Rendón, Albert; Hauert, Roland; Xi, Shibo; Borgna, Armando; Klose, Daniel; Collins, Sean M.; Midgley, Paul A.; Kepaptsoglou, Demie M.; Ramasse, Quentin M.; Ruiz-Ferrando, Andrea; Fako, Edvin; Ortuño, Manuel A.; López, Núria; Carreira, Erick M.; Pérez-Ramírez, Javier
Abstract:	We report the promoting effect of graphitic carbon nitride in Cu-catalyzed N-arylation. The abundance of pyridinic coordination sites in this host permits the adsorption of copper iodide from the reaction medium. The key to achieving high activity is to confine active Cu species on the surface, which is accomplished by introducing atomically dispersed metal dopants to block diffusion into the bulk of the carrier. The alternative route of incorporating metal during the synthesis of graphitic carbon nitride is ineffective as Cu is thermodynamically more stable in inactive subsurface positions. A combination of X-ray absorption, X-ray photoelectron, and electron paramagnetic resonance spectroscopy, density functional theory, and kinetic Monte Carlo simulations is employed to determine the location and associated geometry as well as the electronic structure of metal centers. N-Arylation activity correlates to the surface coverage by copper, which varies during the reaction due to an interplay between site formation via adsorption from the reaction medium and deactivation by diffusion into the bulk of the material, and is highest when an Fe dopant is used to hinder such movement through the lattice.
Fecha de creación:	28-08-2020
Materia(s):	54
Derechos:	L'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/
Páginas:	11069 p.
Tipo de documento:	Artículo Artículo - Versión aceptada
DOI:	doi.org/10.1021/acscatal.0c03164
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