Abstract
Construction of {M4O4} motifs is an effective design paradigm for molecular polyoxometalate- and oxide-based water oxidation catalysts (WOCs). However, the mechanisms beneath this bioinspired design strategy remain a topic of intense debate. The two modifications of LiCoO2 with spinel-type and layer structures are exceptionally versatile model systems to explore the correlations among structure, electronic properties, and photochemical water oxidation. The electronic properties of both LiCoO2 modifications are tunable through delithiation while the basic structural frameworks are maintained. This provides a unique opportunity to assign the respective influence of structures and electronic properties on the water oxidation properties. While spinel-type LiCoO2 with {Co4O4} cubane motifs is active for photochemical water oxidation, the layered modification without cuboidal structural elements is nearly inactive. Here, we demonstrate that the water oxidation performance of both modifications can be significan...
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