Theoretical design of stable hydride clusters: isoelectronic transformation in the EnAl4−nH7+n − series
Cargando...
Archivos
Fecha
2017
Profesor/a Guía
Facultad/escuela
Idioma
en
Título de la revista
ISSN de la revista
Título del volumen
Editor
ROYAL SOC CHEMISTRY
Nombre de Curso
Licencia CC
Licencia CC
Resumen
New stable hydrogen-rich metallic hydrides are designed by systematic transformations of the stable known Al4H7 − species, carried out by successive isoelectronic substitutions of one aluminum atom by one E-H unit at a time (where E = Be, Mg, Ca, Sr and Ba atoms). Searches on the potential energy surfaces (PESs) of EAl3H8 −, E2Al2H9 −, E3AlH10 − and E4H11 − systems indicate that structural analogues of Al4H7 − become higher energy isomers as the number of E-H units increases. The electronic descriptors: Vertical Electron Affinity (VEA), Vertical Ionization Potential (VIP) and the HOMO-LUMO gap, suggest that the systems composed of EAl3H8 −, E2Al2H9 −, E3AlH10 −, with E = Be and Mg, would be the most stable clusters. Additionally, for a practical application, we found that the Be-H and Mg-H substitutions increase the hydrogen weight percentage (wt%) in the clusters, compared with the isoelectronic analogue Al4H7 −. The good capacity of beryllium and magnesium to stabilize the extra hydrogen atoms is supported by the increment of the bridge-like E-H-Al, 3center-2electron chemical bonds. Finally, explorations on the PESs of the neutral species (using Na+ as counterion) indicate that the NaBe2Al2H9, NaBe3AlH10 and NaMg3AlH10 minimum-energy structures retain the original geometric shapes of the anionic systems. This analysis supports the potential use of these species as building blocks for cluster-assembled hydrides in the gas phase.
Notas
Indexación: Web of Science; Scopus.
Palabras clave
Genetic-Algorithm Gega, Gaussian-Basis Sets, Hydrogen storage, Drogen storage, Assembled materials, Atoms LI, Energies, ALNHN+2, Alanes, Series, KR
Citación
RSC Advances Volume 7, Issue 26, 2017, Pages 16069-16077