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2). 2 (c) (e) DFT-optimised molecular structures: (a) Y3C2@C78-D3h (5); (b) Y3C2@C78C2(22010); (c) Y3@C80-Ih(7); (d) Y3C2@C96-D2(186); (e) Y3@C98-C2(166) (ref. 36). Copyright r 2010, American Chemical Society. 18 Chapter 2 52 nitrogen gas as the nitrogen source. The crystallographic data could not locate the speciﬁc position of N but the DFT calculation suggested that the N atom is located at a 665 site, symmetrically between the two metal atoms. The EPR study of Y2@C79N showed that there is a considerable amount of spin density localised on the two equivalent yttrium nuclei.
The HOMO of Sc4(m3-O)2@Ih-C80 is delocalised over the four Sc ions. The analysis of atomic charges shows that this metallic oxide EMF has a special mixed-valence cluster that gives rise to an electronic structure of (Sc2,331)2(Sc1,421)2(O2–)2@(Ih-C80)6–. For Sc4(m3-O)3@Ih-C80, however, the HOMO is localised on the carbon cage and the LUMO is localised on the metal cluster, which resembles that of Sc3N@Ih-C80. The additional third oxygen atom in the cluster of Sc4(m3-O)3@Ih-C80 gives rise to four fully oxidised Sc ions with an oxidation state of 3 þ compared with the mixed-valence cluster in the Sc4(m3-O)2@Ih-C80.
97 This is presumably due to the similar electronic structures of Pr, Nd and Ce. The electrochemistry of Nd3N@C96, Pr3N@C96 and Ce3N@C96 were also studied. 7 Metallic Oxide EMFs Oxygen had been long viewed as a must-be-avoided gas in the arcing process and considered to have adversely aﬀected the formation of endohedral fullerenes. However, Stevenson et al. 17,127,128 The increasing ﬂow rate of air improved the production of metallic oxide EMFs. 127 Sc4O3@C80 shows the entrapment of a seven-atom cluster into the carbon cage that is, by far, the largest encapsulated cluster ever found inside a fullerene carbon cage.