Many important redox reactions involve transfer of both protons and electrons. One example is the electrocatalytic reduction of O2 to water, the oxygen reduction reaction (ORR). New catalysts and model systems for the ORR are being developed using proton relays to deliver H+ to oxygen intermediates.  In one approach, we have prepared a new class of tripodal ligands incorporating pendant tertiary amines, which is both modular and flexible. Various metal complexes these amines are being tested for ORR activity. Iron porphyrin catalysts with 2-carboxyphenyl substituents have been found to be active and selective ORR catalysts, and the proton relays seem to be important.  In parallel with these molecular cmplexes, interfacial redox reactions of ZnO and TiO2 nanoparticles are being examined.  Various experiments indicate that reduced forms of these particles can react by proton-coupled electron transfer (PCET), not just by electron transfer.  The implications of these results will be discussed.

Focusing on protons in catalytic and interfacial redox reactions

243rd National Meeting (2012)

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