The efficient interconversion of electrical and chemical energy requires catalysts capable of accelerating complex multi-electron reactions at electrified interfaces. Meeting this goal requires new methods of controlling the structure of electrode surface active sites at the molecular level. We have developed a simple method for attaching molecules to graphitic carbon electrodes through conjugated aromatic pyrazine linkages. The resulting graphite-conjugated catalysts (GCCs) are active for oxygen and carbon dioxide reduction catalysis and spectroscopic studies indicate that the conjugated linkage leads to strong electronic coupling between GCC sites and the graphitic electrode. In particular, the conjugated molecules behave like metallic surface sites, providing a unique opportunity to investigate heterogeneous electrochemical reactivity with molecular precision. Our latest efforts to develop and investigate this tunable class of molecularly well-defined heterogeneous catalysts will be discussed.

Molecular approaches to heterogeneous electrocatalysis

255th National Meeting (2018)

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