title: Promoting Photochemical Water Oxidation with Metallic Band Structures.
abstract: The development of economic water oxidation catalysts is a key step toward large-scale water splitting. However, their current exploration remains empirical to a large extent. Elucidating the correlations between electronic properties and catalytic activity is crucial for deriving general and straightforward catalyst design principles. Herein, strongly correlated electronic systems with abundant and easily tunable electronic properties, namely La(1-x)Sr(x)BO3 perovskites and La(2-x)Sr(x)BO4 layered perovskites (B = Fe, Co, Ni, or Mn), were employed as model systems to identify favorable electronic structures for water oxidation. We established a direct correlation between the enhancement of catalytic activity and the insulator to metal transition through tuning the electronic properties of the target perovskite families via the La(3+)/Sr(2+) ratio. Their improved photochemical water oxidation performance was clearly linked to the increasingly metallic character. These electronic structure-activity relations provide a promising guideline for constructing efficient water oxidation catalysts.
authors.affiliation: Department of Chemistry, University of Zurich , Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.
authors.forename: Hongfei
authors.initials: H
authors.lastname: Liu
authors.affiliation: Department of Chemistry, University of Zurich , Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.
authors.forename: René
authors.initials: R
authors.lastname: Moré
authors.affiliation: Physics Institute, University of Zurich , Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.
authors.forename: Henrik
authors.initials: H
authors.lastname: Grundmann
authors.affiliation: Department of Chemistry, University of Zurich , Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.
authors.forename: Chunhua
authors.initials: C
authors.lastname: Cui
authors.affiliation: Electron Microscopy Center, Empa, Swiss Federal Laboratories for Materials Science and Technology , Überlandstrasse 129, CH-8600 Dübendorf, Switzerland.
authors.forename: Rolf
authors.initials: R
authors.lastname: Erni
authors.affiliation: Department of Chemistry, University of Zurich , Winterthurerstrasse 190, CH-8057 Zurich, Switzerland.
authors.forename: Greta R
authors.initials: GR
authors.lastname: Patzke