Interfacing earth-abundant electrocatalysts with mesostructured oxide photoanodes for solar photoelectrocatalysis.

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With this award from the Chemical Catalysis Program of the Chemistry Division of the National Science Foundation, Professor Daniel Gamelin at the University of Washington, Seattle, will carry out studies in the area of solar energy conversion and storage in the form of chemical fuels. Specifically, this project seeks to address the challenge of interfacing non-crystalline water-oxidation electrocatalysts with crystalline semiconductor photoelectrodes for photolectrochemical (PEC) solar energy conversion. The research will use a combination of preparative and analytical techniques to develop a deeper understanding of interfaces in a set of composite catalyst/semiconductor photoanodes. The principal investigator (PI) will apply state-of-the-art photoelectrochemical and spectroscopic techniques to assay these photoelectrodes and to advance understanding of microscopic relationships between surface morphology, functionalization, and redox catalysis. The PI and his team will seek to develop fundamental structure/function relationships that address catalyst-semiconductor coupling, electron-hole recombination dynamics, and the impact such catalysts have on the photoanode electronic structure. The research will address mechanistic differences between electrocatalytic and photoelectrocatalytic responses of this family of water-oxidation catalysts, as well as performance differences. This work will improve the solar water splitting efficiencies of these composite photoanodes in PEC cell configurations, particularly at low overpotentials where recombination losses are most severe and detrimental to energy conversion efficiencies.This research will focus on interfacing non-crystalline Earth-abundant electrocatalysts with mesostructured oxide photoanodes for use in solar photoelectrochemical devices capable of splitting water that will generate hydrogen as a chemical fuel. This research will advance the general understanding of such composite photoelectrodes for photoelectrochemical solar energy conversion. The research will yield new complex materials and new fundamental knowledge that could broadly impact future alternative-energy technologies. This project will also provide advanced interdisciplinary training in the areas of inorganic, physical, electro-, and materials chemistries, in order to prepare participating undergraduates, graduate students, and postdoctoral researchers for future careers in science, engineering, and education. There is a special emphasis on integration of research and education at the early career levels (undergraduate, high school) through aggressive involvement of undergraduates, incorporation of experiments and concepts from this research into the University of Washington undergraduate curriculum, collaboration with faculty and students from undergraduate institutions, and mature outreach activities at Seattle-area high schools and community colleges.