This presentation will focus on the coupling of semiconductor nanocrystals as light absorbers with redox catalysts for multi-electron transfer reactions to drive solar photochemistry. Reactions of interest include H2 generation, CO2 reduction, N2 fixation, and water oxidation. This presentation will summarize how nanocrystal excited state behavior and surface chemistry impact the rates and efficiencies of photoexcited electron transfer from CdS nanorods to the enzyme hydrogenase, which catalyzes proton reduction to H2. A combination of transient absorption spectroscopy and kinetic modeling allowed us to quantitatively understand the competition between electron transfer and the excited state relaxation processes in the CdS nanorods, and the relationship between these processes and the overall photochemical H2 formation. These insights will then be applied to a more catalytically complex system: CdS nanorods complexed with an oxidoreductase that catalyzes formation of carbon-carbon bonds via CO2 reduction. The presentation will feature our most recent results on charge transfer between semiconductor nanocrystals and redox enzymes.

Elucidating how photoexcited semiconductor nanocrystals drive redox enzyme catalysis

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.