was successfully synthesized and isolated by multistage HPLC for the first time. All of these isolated metallofullerenes were confirmed by LD-TOF mass spectrometry and characterized by UV-vis-NIR absorption spectroscopy. The valence state of the encaged ytterbium atoms, the probable molecular symmetries, and the electronic structures are discussed in terms of their HPLC behaviors and absorption spectra. In particular, two new mono-metallofullerene isomers based on C 74 and C 84 cages were isolated for the first time that are proposed to have completely novel cage structures not reported elsewhere so far.

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The electrochemical properties of a series of metallofullerenes with different cages, namely, Yb@C74(II), Yb@C76(I, II), Yb@C78, Yb@C80, Yb@C82(I, II, III), and Yb@C84(II, III, IV), have been systematically investigated by cyclic and differential pulse voltammetry experiments for the first time. This article discusses the electronic structures of these metallofullerenes based on the results from these experiments. From previous electrochemical work and the above discussion, it is concluded that the nondegenerate LUMO is a common characteristic of the electronic structures of the higher fullerenes and monometallofullerenes. In addition, the effect of the cage on the electronic structure and properties of the metallofullerene is estimated from the plot of the reduction potential versus the carbon number of the metallofullerene. This estimation shows that usually the electronic structure and properties of the metallofullerene vary with cage size and structure. The cage structure is of particular importance for determining the electronic structure and properties. Moreover, an explanation concerning the abundance and stability of C82-based trivalent monometallofullerenes is given from an electronic structural standpoint.