title: Water Oxidation Mechanisms of Metal Oxide Catalysts by Vibrational Spectroscopy of Transient Intermediates.
abstract: Water oxidation is an essential reaction of an artificial photosystem for solar fuel generation because it provides electrons needed to reduce carbon dioxide or protons to a fuel. Earth-abundant metal oxides are among the most attractive catalytic materials for this reaction because of their robustness and scalability, but their efficiency poses a challenge. Knowledge of catalytic surface intermediates gained by vibrational spectroscopy under reaction conditions plays a key role in uncovering kinetic bottlenecks and provides a basis for catalyst design improvements. Recent dynamic infrared and Raman studies reveal the molecular identity of transient surface intermediates of water oxidation on metal oxides. Combined with ultrafast infrared observations of how charges are delivered to active sites of the metal oxide catalyst and drive the multielectron reaction, spectroscopic advances are poised to play a key role in accelerating progress toward improved catalysts for artificial photosynthesis.
authors.affiliation: Chemical Sciences Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, California 94720; email: mzhang@lbl.gov.
authors.forename: Miao
authors.initials: M
authors.lastname: Zhang
authors.affiliation: Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, University of California, Berkeley, California 94720; email: hmfrei@lbl.gov.
authors.forename: Heinz
authors.initials: H
authors.lastname: Frei
keywords: artificial photosynthesis; infrared and Raman spectroscopy; metal oxides; surface intermediates; transients; water oxidation catalysis