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Photosynthetic water oxidation is catalyzed by a Mn 4 O 5 Ca cluster with an unprecedented arrangement of metal ions in which a single manganese center is bonded to a distorted Mn 3 O 4 Ca cubane-like structure. Several mechanistic proposals describe the unique manganese center as a site for water binding and subsequent formation of a high valent Mn-oxo center that reacts with a M-OH unit (M = Mn or Ca II ) to form the O-O bond. The conversion of low valent Mn-OH n (n = 1,2) to a Mn-oxo species requires that a single manganese site be able to accommodate several oxidation states as the water ligand is deprotonated. To study these processes, the preparation and characterization of a new monomeric Mn IV -OH complex is described. The Mn IV -OH complex completes a series of well characterized Mn-OH and Mn-oxo complexes containing the same primary and secondary coordination spheres; this work thus demonstrates that a single ligand can support mononuclear Mn complexes spanning four different oxidation states (II through V) with oxo and hydroxo ligands that are derived from water. Moreover, we have completed a thermodynamic analysis based on this series of manganese complexes to predict the formation of high valent Mn-oxo species; we demonstrated that the conversion of a Mn IV -OH species to a Mn V -oxo complex would likely occur via a stepwise proton transfer-electron transfer mechanism. The large dissociation energy for the Mn IV O-H bond (~95 kcal/mol) diminished the likelihood that other pathways are operative within a biological context. Furthermore, these studies showed that reactions between Mn-OH and Mn-oxo complexes lead to non-productive, one-electron processes suggesting that initial O-O bond formation with the OEC does not involve an Mn-OH unit.

chemical science

Preparation and properties of an Mn<sup>IV</sup>–hydroxide complex: proton and electron transfer at a mononuclear manganese site and its relationship to the oxygen evolving complex within photosystem II

Preparation and properties of an MnIV–hydroxide complex: proton and electron transfer at a mononuclear manganese site and its relationship to the oxygen evolving complex within photosystem II

Preparation and properties of an Mn^IV–hydroxide complex: proton and electron transfer at a mononuclear manganese site and its relationship to the oxygen evolving complex within photosystem II