Computational exploration of NO single-site disproportionation on Fe-MOF-5

Nitric oxide disproportionation at the site-isolated Fe centers of the metal organic framework material known as Fe-MOF-5 has been explored with density functional theory (DFT). The computed reaction sequence supports the mechanism suggested by experiment that involves the formation of the monoanion...

Descripción completa

Detalles Bibliográficos
Autores: Jover Modrego, Jesús, Brozek, Carl K., Dincă, Mircea, López, Núria (López Alonso)
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2019
País:España
Institución:Varias* (Consorci de Biblioteques Universitáries de Catalunya, Centre de Serveis Científics i Acadèmics de Catalunya)
Repositorio:Recercat. Dipósit de la Recerca de Catalunya
OAI Identifier:oai:recercat.cat:2445/149340
Acceso en línea:https://hdl.handle.net/2445/149340
Access Level:acceso abierto
Palabra clave:Ferro
Reaccions químiques
Energia
Metalls de transició
Iron
Chemical reactions
Energy
Transition metals
Descripción
Sumario:Nitric oxide disproportionation at the site-isolated Fe centers of the metal organic framework material known as Fe-MOF-5 has been explored with density functional theory (DFT). The computed reaction sequence supports the mechanism suggested by experiment that involves the formation of the monoanionic hyponitrite radical. The validity of the computed reaction mechanism is bolstered by impressive agreement between computed and experimental vibrational spectroscopic evidence of each reaction step. Similarly the analogous MnII-MOF-5 system indicates that the disproportionation of NO should proceed smoothly with this single-site material. These results, observed also for some homogeneous Mn(II) catalysts, indicate that heterogeneous Mn-based materials could be employed as efficient biological and industrial catalytic systems in NO disproportionation processes.