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Octahedral Hexapalladium Pseudo- T d Pd 6 (μ 3 -CO) 4 (PEt 3 ) 6 with 80 Electron-Deficient Cluster Valence Electrons (CVEs) and a Comparison with Octahedral Hexapalladium Pseudo- C 2 v Pd 6 (μ 3 -CO) 4 (PMe 3 ) 7 with 82 CVEs: Computational Analysis and Resulting Implications.
Inorganic Chemistry 2022 December 17
The elusive octahedral hexapalladium Pd6 (μ3 -CO)4 (PEt3 )6 ( 1 ) was obtained by the reaction of Pd10 (CO)12 (PEt3 )6 with TlCo(CO)4 in tetrahydrofuran under N2 at 55 °C. Its pseudo- T d octahedral structure, established from a CCD X-ray diffractometry study at 100 K, has the highest ideal symmetry of any of the characterized octahedral-based CO/PR3 -ligated homopalladium Pd n clusters ( n = 6, 7, 8, 10). Each Pd atom in 1 is coordinated to a PEt3 ligand, and each nonadjacent triangular Pd3 face is capped by a triply bridging μ3 -CO ligand. The 31 P{1 H} NMR and IR spectra of 1 are in accordance with its solid-state molecular structure. Cluster 1 has a total of 80 cluster valence electrons (CVEs), the lowest reported for octahedral-based metal polyhedra that normally conform to the Wade-Mingos bonding rule with an 86 CVE count. Comparative density functional theory calculations involving natural population analysis are presented for trimethylphosphine analogues of the triethylphosphine ( 1-Me ) and the previously reported octahedral hexapalladium trimethylphosphine Pd6 (μ3 -CO)4 (PMe3 )7 ( 2 ), which has pseudo- C 2 v symmetry with 82 total CVEs.
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