Colloidal nanocrystals (NCs) are attractive chromophores for homogenous single- and multi-electron photoredox reactions. NCs are typically grown by precipitation from high-boiling organic solvents in the presence of organic surfactant molecules that permit surface stabilization, size control, and processability in non-polar liquids. The bulky surfactants that are required for NC synthesis, however, also prevent co-catalysts, substrates, and other molecules from accessing the NC surface, which limits the applicability of NCs in photocatalysis. The native surfactants should be replaced with more compact organic/inorganic molecules that permit attachment of substrate and/or co-catalyst molecules to the NC surface while maintaining the colloidal stability required to suspend the NCs in solution. Here, we present surface modification strategies for functionalizing NCs with transition metal co-catalysts that have the potential to exchange and store multiple photoexcited charges with the NC.  Emergent properties in the NC-molecule assemblies are spectroscopically characterized, including their dependence on the quantity of surface adsorbates. The hybrid nanocrystal-molecule architectures targeted here are expected to have photophysical attributes that are of interest for catalyzing environmentally and industrially relevant redox reactions.

Attachment of molecular catalysts to nanocrystal surfaces facilitated by anionic bridging ligands

255th National Meeting (2018)

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