The oxygen reduction reaction (ORR) is the major source of overpotential loss in low-temperature fuel cells. Pt-based materials have been found to be the most effective electrocatalysts, but exploration of alternatives has been hampered by stability constraints at the typical operating conditions of low pH and high potential. I will discuss our studies of elementary mechanism of ORR on various metal electrodes using kinetic and micro-kinetic analysis of reaction pathways and quantum chemical calculations as well as surface enhanced Raman spectroscopic (SERS). These studies allowed us to identify the elementary steps and molecular descriptors that govern the rate of ORR. Using these performance descriptors, we have been able to identify families of Pt-based alloys that exhibit superior ORR performance is acid and base respectively. We have synthesized these alloys to demonstrate the superior ORR activity with rotating disk electrode experiments. We have also performed thorough structural characterization of the bulk and surface properties with a combination of cyclic voltammetry, x-ray diffraction, and electron microscopy with spatially resolved energy-dispersive x-ray spectroscopy and electron energy loss spectroscopy. Throughout the talk, I will focus on the similarities between application of kinetics and spectroscopy in thermal and electrochemical processes.

From kinetics and spectroscopy to new materials for electrochemical oxygen reduction reaction

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