Popis: |
This report summarizes the three-year LDRD program directed at developing catalysts based on metalloporphyrins to reduce carbon dioxide. Ultimately it was envisioned that such catalysts could be made part of a solar-driven photoredox cycle by coupling metalloporphyrins with semiconductor systems. Such a system would provide the energy required for CO{sub 2} reduction to methanol, which is an uphill 6-electron reduction. Molecular modeling and design capabilities were used to engineer metalloporphyrin catalysts for converting CO{sub 2} to CO and higher carbon reduction products like formaldehyde, formate, and methanol. Gas-diffusion electrochemical cells were developed to carry out these reactions. A tin-porphyrin/alumina photocatalyst system was partially developed to couple solar energy to this reduction process. |