title: Fast water oxidation using iron.
abstract: Photolysis of water, a long-studied strategy for storing solar energy, involves two half-reactions: the reduction of protons to dihydrogen and the oxidation of water to dioxygen. Proton reduction is well-understood, with catalysts achieving quantum yields of 34% when driven by visible light. Water oxidation, on the other hand, is much less advanced, typically involving expensive metal centers and rarely working in conjunction with a photochemically powered system. Before further progress can be made in the field of water splitting, significant developments in the catalysis of oxygen evolution are needed. Herein we present an iron-centered tetraamido macrocyclic ligand (Fe-TAML) that efficiently catalyzes the oxidative conversion of water to dioxygen. When the catalyst is combined in unbuffered solution with ceric ammonium nitrate, its turnover frequency exceeds 1.3 s(-1). Real-time UV-vis and oxygen monitoring of the active complex give insights into the reaction and decay kinetics.
authors.affiliation: Department of Chemistry, Carnegie Mellon University, Pittsburgh, Pennsylvania 15213, USA.
authors.forename: W Chadwick
authors.initials: WC
authors.lastname: Ellis
authors.forename: Neal D
authors.initials: ND
authors.lastname: McDaniel
authors.forename: Stefan
authors.initials: S
authors.lastname: Bernhard
authors.forename: Terrence J
authors.initials: TJ
authors.lastname: Collins