Tandem dye-sensitized photo-electrosynthesis cells require light absorption from both the anodic and the cathodic portions of the cell. Several strategies have been demonstrated to couple a chromophore/redox mediator with a water oxidation catalyst on the anodic side, but few examples exist where the reduction catalyst is bound to a redox mediator or a high valence band semiconductor. Presented here is a versatile approach to couple both water oxidation and proton reduction catalysts to chromophore/redox mediators utilizing amide chemistry. The amide coupling chemistry also allows for the introduction of saturation and length variations between the catalyst and chromophore. These systems can in turn be immobilized on metal oxide surfaces through phosphonic acid functionalities to complete the DSPEC. The observed rate enhancements and lowered overpotentials due to increased electron transfer rates from the catalysts to the redox mediator are also presented.

Synthesis and electrochemical analysis of molecular catalysts for water oxidation and proton reduction bound to chromophore/redox-mediators: Toward tandem dye-sensitized photo-electrosynthesis cells (DSPECs)

243rd National Meeting (2012)

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