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The syntheses of the two novel complexes [Ag{Mo/W(CO) 6 } 2 ] + [F‐{Al(OR F ) 3 } 2 ] −  (R F =C(CF 3 ) 3 ) are reported along with their structural and spectroscopic characterization. The X‐ray structure shows that three carbonyl ligands from each M(CO) 6  fragment bend towards the silver atom within binding Ag−C distance range. DFT calculations of the free cations [Ag{M(CO) 6 } 2 ] +  (M=Cr, Mo, W) in the electronic singlet state give equilibrium structures with  C  2  symmetry with two bridging carbonyl groups from each hexacarbonyl ligand. Similar structures with  C  2  symmetry (M=Nb) and  D  2  symmetry (M=V, Ta) are calculated for the isoelectronic group 5 anions [Ag{M(CO) 6 } 2 ] −  (M=V, Nb, Ta). The electronic structure of the cations is analyzed with the QTAIM and EDA‐NOCV methods, which provide detailed information about the nature of the chemical bonds between Ag +  and the {M(CO) 6 } 2   q   ( q  = −2, M = V, Nb, Ta;  q  = 0, M = Cr, Mo, W) ligands.

chemistry – a european journal

Group 6 Hexacarbonyls as Ligands for the Silver Cation: Syntheses, Characterization, and Analysis of the Bonding Compared with the Isoelectronic Group 5 Hexacarbonylates