Endohedral metallofullerenes have greatly expanded the range of the fullerene family due to their nesting structure and unusual encapsulated clusters protected by a fullerene cage. Herein, we report a metallofullerene ScCNH@-C, which has a scandium tetrahedron supported by H and CN anions inside fullerene C. ScCNH@-C has a rare multilayer nesting structure, and the internal ScCNH is the most complex endohedral cluster disclosed to date. ScCNH@-C has so many bonding types (metal-carbide, metal-nitride, and metal-hydride), which weave a polyhedron of ScCNH clusters. This work shows that the endohedral metallofullerenes have the potential to build inorganic nesting polyhedra that have distinctive architectures and unique electronic properties. ScCNH@-C was synthesized by means of the arc-discharge method using scandium and graphite under the mixed atmosphere of hydrogen, nitrogen, and helium. It is the first time to disclose an unprecedented metal-hydride bond in a fullerene cage. This result shows that the endohedral fullerenes bearing hydrogen species can be synthesized by the arc-discharge technique under an atmosphere of hydrogen. This work demonstrates that a fullerene cage can be an ample carrier to encapsulate unusual cluster moieties.
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