Water-splitting photoelectrochemical cells suffer from very low efficiencies, in large part due to charge recombination processes, which outcompete the desired redox reactions. In this study, we set out to retard the rate of charge transfer from an oxidized catalytic metal center to the anode surface that the catalyst is covalently attached to. To this end, a rigid, polycyclic, aliphatic linker molecule was synthesized from commercially available pregnenolone in five steps. The linker was then used to covalently attach a catalytically active iridium species to the surface of a mesoporous metal oxide semiconductor film. <i>Ab initio </i> quantum calculations were used to predict the rates of recombination for this species, as well as multiple synthetically viable analogs.

Iridium on Steroids: using rigid, polycyclic, aliphatic molecules as non-conductive linkers to bind catalytic centers to metal oxide semi-conductors

254th National Meeting (2017)

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