Although surface-immobilized molecular electrocatalysts show promise for the selective electroreduction of energy-relevant small molecules to useful products, a significant impediment to their implementation is their low activity per geometric area compared to heterogeneous analogues. This difference is due to the fact that well-defined films of surface-immobilized molecular catalysts are often limited to monolayer coverages, whereas solid-state materials often have 3-D architectures affording them many more active sites per geometric area. To address this limitation, we have developed a layer-by-layer strategy for the synthesis of well-defined multilayer films of discrete molecular catalysts. In this way, we form 3-D catalyst architectures that maintain the selectivity of molecular catalysts, but operate with the increased activity per geometric area. We have explored these multilayer systems for electrocatalytic O<sub>2</sub> reduction and selective CO<sub>2</sub> reduction.

Layer-by-layer growth of molecular catalyst films for the electrocatalytic reduction of small molecules

254th National Meeting (2017)

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