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Proton-responsive half-sandwich Cp*Ir(III) complexes possessing a bipyridine ligand with two hydroxy groups at the 3,3′-, 4,4′-, 5,5′-, or 6,6′-positions (3DHBP, 4DHBP, 5DHBP, or 6DHBP) were systematically investigated. UV–vis titration data provided average pKa values of the hydroxy groups on the ligands. Both hydroxy groups were found to deprotonate in the pH 4.6–5.6 range for the 4–6DHBP complexes. One of the hydroxy groups of the 3DHBP complex exhibited a low pKa value of <0.4 because the deprotonation is facilitated by the strong intramolecular hydrogen bond formed between the generated oxyanion and the remaining hydroxy group, which in turn leads to an elevated pKa value of ∼13.6 for the second deprotonation step. The crystal structures of the 4- and 6DHBP complexes obtained from basic aqueous solutions revealed their deprotonated forms. The intramolecular hydrogen bond in the 3DHBP complex was also observed in the crystal structures. The catalytic activities of these complexes in aqueous phase reac...

Positional Effects of Hydroxy Groups on Catalytic Activity of Proton-Responsive Half-Sandwich Cp*Iridium(III) Complexes