(Invited) Water Oxidation Catalysis with Atomically Defined Active Sites on Nanostructured Materials for Solar Energy Applications

Abstract

Devising cost effective methods for efficiently capturing and storing solar energy is among the grand challenges of science (1). We are using insights from studies of natural photosynthetic systems (2) to develop bioinspired materials for photo-electrochemical water oxidation and solar fuel production by using molecular catalysts and dyes attached to mesoporous metal oxide photoanodes. Molecular catalysts are known for their high activity and tunability, but their solubility and limited stability often restrict their use in practical applications. We are developing anchoring chemistry to attach molecular water-oxidation catalysts to metal oxide surfaces (3), which not only greatly increases the stability of the molecular catalyst but also improves the catalytic performance of the oxide material. Our progress on the development and characterization of molecular iridium, copper and manganese water-oxidation catalysts (4-5), along with their application for photoelectrochemical water oxidation (6) and solar fuel production, will be discussed. Directing Matter and Energy: Five Challenges for Science and the Imagination, U.S. Department of Energy, Washington, DC, December 2007.D.J. Vinyard and G.W. Brudvig, Annu. Rev. Phys. Chem. (2017) 68, 101.J.L. Troiano, R.H. Crabtree and G.W. Brudvig, ACS Appl. Mater. Interfaces (2022) 14, 6582.S.W. Sheehan et al., Nature Comm. (2015) 6, 6469.K.J. Fisher et al., ACS Catalysis (2017) 7, 3384.Y. Zhao et al., Proc. Natl. Acad. Sci. U.S.A. (2018) 115, 2902.