Theoretical design of stable hydride clusters: isoelectronic transformation in the EnAl4−nH7+n series

Carolina Giraldo, Franklin Ferraro, C. Z. Hadad, Lina Riuz, William Tiznado, Edison Osorio

Resultado de la investigación: Article

1 Cita (Scopus)

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.

Idioma originalEnglish
Páginas (desde-hasta)16069-16077
Número de páginas9
PublicaciónRSC Advances
Volumen7
N.º26
DOI
EstadoPublished - 1 ene 2017

Huella dactilar

Hydrides
Hydrogen
Potential energy surfaces
Atoms
Substitution reactions
Beryllium
Electron affinity
Ionization potential
Chemical bonds
Aluminum
Isomers
Magnesium
Gases

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Citar esto

Giraldo, Carolina ; Ferraro, Franklin ; Hadad, C. Z. ; Riuz, Lina ; Tiznado, William ; Osorio, Edison. / Theoretical design of stable hydride clusters : isoelectronic transformation in the EnAl4−nH7+n series. En: RSC Advances. 2017 ; Vol. 7, N.º 26. pp. 16069-16077.
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title = "Theoretical design of stable hydride clusters: isoelectronic transformation in the EnAl4−nH7+n − series",
abstract = "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.",
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doi = "10.1039/c7ra01422h",
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Theoretical design of stable hydride clusters : isoelectronic transformation in the EnAl4−nH7+n series. / Giraldo, Carolina; Ferraro, Franklin; Hadad, C. Z.; Riuz, Lina; Tiznado, William; Osorio, Edison.

En: RSC Advances, Vol. 7, N.º 26, 01.01.2017, p. 16069-16077.

Resultado de la investigación: Article

TY - JOUR

T1 - Theoretical design of stable hydride clusters

T2 - isoelectronic transformation in the EnAl4−nH7+n − series

AU - Giraldo, Carolina

AU - Ferraro, Franklin

AU - Hadad, C. Z.

AU - Riuz, Lina

AU - Tiznado, William

AU - Osorio, Edison

PY - 2017/1/1

Y1 - 2017/1/1

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85015414824&partnerID=8YFLogxK

U2 - 10.1039/c7ra01422h

DO - 10.1039/c7ra01422h

M3 - Article

AN - SCOPUS:85015414824

VL - 7

SP - 16069

EP - 16077

JO - RSC Advances

JF - RSC Advances

SN - 2046-2069

IS - 26

ER -