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N-2(-) radical anion reversibly formed at the surface of "electron-rich" alkaline-earth oxides

Giamello, Elio, Paganini, Maria Cristina, Chiesa, Mario, Murphy, Damien Martin, Pacchioni, Gianfranco, Soave, Raffaella and Rockenbauer, Antal 2000. N-2(-) radical anion reversibly formed at the surface of "electron-rich" alkaline-earth oxides. Journal of Physical Chemistry B 104 (9) , pp. 1887-1890. 10.1021/jp994126y

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Physisorption of N2 gas onto the surface of a metal oxide (MgO or CaO), containing paramagnetic trapped electron centers (FS + color centers), leads to the formation of a paramagnetic species that, on the basis of its EPR spectrum and of the related spin-Hamiltonian parameters, is identified as a N2 - radical anion. The species in fact contains two nitrogen atoms and its g and A tensors are in agreement with what observed for the N2 - radical trapped in irradiated crystal of various azides. The surface N2 - species is formed by surface-tomolecule one-electron transfer, and its stability strictly parallels the stability of the physisorbed layer, the species formation being completely reversible and pressure dependent. When the N2 adlayer is desorbed, in fact, the N2 - spectrum vanishes and the original Fs + spectrum is restored. Ab initio quantum chemical calculations on an embedded MgO cluster fully confirm the observed phenomenon indicating, in agreement with EPR analysis, the electron transfer of a large fraction of electron density into the ð orbitals of the admolecule.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Chemistry
Subjects: Q Science > QD Chemistry
Publisher: American Chemical Society
ISSN: 0022-3654
Last Modified: 04 Jun 2017 05:06

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