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The removal of H atoms from polyhedral boranes results in the formation of dangling radial orbitals with one electron each. If there is a requirement of electrons for skeletal bonding to meet the Wade's rule, these are provided from the exohedral orbitals. Additional electrons occupy a linear combination of the dangling orbitals. Stabilization of these molecular orbitals depends on their overlap. The lateral (sideways) overlap of dangling orbitals decreases with the decreasing cluster size from 12 to 5 boron atoms as the orbitals become more and more splayed out. Thus, as the number of dangling orbitals increases, the destabilization of their combinations increases at a higher rate for smaller polyhedral boranes, leading to flat structures with the removal of a fewer number of hydrogens. Though exohedral orbitals form better overlap in larger polyhedral clusters, the increase of electrons with the removal of H atoms results in occupancy of antibonding skeletal orbitals (beyond Wade's rules) and leads to flat structures. The reverse happens when hydrogens are added to a flat cluster. Substitution of BH by Si does not change structural patterns.

inorganic chemistry

Overlap of Radial Dangling Orbitals Controls the Relative Stabilities of Polyhedral BnHn–x Isomers (n = 5–12, x = 0 to n – 1)