Dedicated to the memory of Professor Robert Vleggaar is investigated by means of cyclic voltammetry. The complexes all exhibit a twoelectron oxidation process that is W-based and a one-electron reduction that is mainly localized on the carbene ligand. Complexes 1-4 and 9-12 are considerably more difficult to oxidize than 5-8 due to the better π-acceptor ability of the (CO) 4 (PR' 3 ) (R' = Ph or OPh) ligand combination than that of (CO) 3 (dppe). Density functional theory calculations on the neutral, reduced and oxidized complexes confirmed the role of the frontier orbitals in the oxidation and reduction processes and enabled formulation of mathematical relationships that can be used to predict experimental measured potentials. X-ray crystal structures of 2cis, 3 and 5 are discussed.

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