Εξειδίκευση τύπου :	Άρθρο σε επιστημονικό περιοδικό
Τίτλος:	Theoretical investigation of the interaction of CH4 with Al-2 and Al-3 neutral and charged clusters
Δημιουργός/Συγγραφέας:	Alexandrou, E. I. Gross, A. [EL] Μπακάλης, Ναούμ Χ.[EN] Bacalis, Naoum C.
Εκδότης:	American Institute of Physics
Τόπος έκδοσης:	MELVILLE
Ημερομηνία:	2010-04-21
Γλώσσα:	Αγγλικά
ISSN:	0021-9606
DOI:	10.1063/1.3376174
Περίληψη:	We have studied the interaction of CH4 with Al-2 and Al-3 neutral and charged clusters in the two lowest lying spin states using density functional theory. These calculations, via extended search, are used to determine the stable positions of H and CH3 near the cluster, and the transition state to break the H-CH3 bond. In all cases, stable methyl-aluminum-hydrides are possible. The H desorption is studied by means of vibration analysis and application of transition state theory. A common observed trend is that, in breaking the H-CH3 bond, the interacting H atom is attached to the "surface" of the clusters attracting some negative charge of approximate to 0.2e. The charge transfer is illustrated using the corresponding orbitals near the transition state in conjunction with the computed Mulliken population analysis. Thermal vibrations, generally, do not enhance the reaction. In all exothermic cases, the binding energy toward CH3+HAlncharge increases with increasing charge of the original Al-n((q=-1,0,1)) cluster. Although Al lacks occupied d-orbitals, the small Al clusters reduce the (free methane) CH3-H dissociation barrier except for Al-3((q=-1,0)). The relevant reactions in desorption require similar to 400-700 degrees C.
Τίτλος πηγής δημοσίευσης:	Journal of Chemical Physics
Τόμος/Κεφάλαιο:	132
Τεύχος:	15
Σελίδες:	[14]
Θεματική Κατηγορία:	[EL] Φυσική[EN] Physics
Λέξεις-Κλειδιά:	aluminium atomic clusters atom-molecule reactions binding energy bonds (chemical) charge exchange density functional theory desorption dissociation ion-molecule reactions metal clusters organic compounds reaction kinetics theory vibrational states Physics, Atomic, Molecular & Chemical
Αξιολόγηση από ομότιμους (peer reviewed):	Ναι
Κάτοχος πνευματικών δικαιωμάτων:	© AMER INST PHYSICS
Ηλεκτρονική διεύθυνση περιοδικού (link) :	http://jcp.aip.org/jcp/staff.jsp
Εμφανίζεται στις συλλογές:	Ινστιτούτο Θεωρητικής και Φυσικής Χημείας (ΙΘΦΧ) - Επιστημονικό έργο