The goal of our DOE-supported research has been to explore the use of solid state materials as organizing media for, and as active components of, artificial photosynthetic systems. In this work we strive to understand how photoinduced electron and energy transfer reactions occur in the solid state, and to elucidate design principles for using nanoscale inorganic materials in photochemical energy conversion schemes. A unifying theme in this project has been to move beyond the study of simple transient charge separation to integrated chemical systems that can effect permanent charge separation in the form of energy-rich chemicals. This project explored the use of zeolites as organizing media for electron donor-acceptor systems and artificial photosynthetic assemblies. Layer-by-layer synthetic methods were developed using lamellar semiconductors, and multi-step, visible light driven energy/electron transfer cascades were studied by transient specroscopic techniques. By combining molecular photosensitizers with lamellar semiconductors and intercalated catalyst particles, the first non-sacrificial systems for visible light driven hydrogen evolution were developed and studied. Oxygen evolving catalyst particles and semiconductor nanowires were also studied with the goal of achieving photocatalytic water splitting using visible light.

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