Abstract
This chapter explores the polyhedral skeletal electron pair theory (PSEPT), which relates the three-dimensional structures of polyhedral molecules to the total number of valence electrons. It represents an analogue of the valence shell electron pair (VSEPR) theory for three-dimensional cage molecules. The simplest three-dimensional cage structures have each vertex connected to three other vertices. The chapter then illustrates some typical three-connected polyhedral skeletal geometries. Such molecules may be described using conventional two-centre two-electron bonding schemes based on the effective atomic number rule. The chapter also looks at transitional metal polyhedral molecules and electron-rich clusters..
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