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Precious-metal-free spinel oxide electrocatalysts are promising candidatesfor catalyzing the oxygen reduction reaction (ORR) in alkaline fuel cells. Inthis theory-driven study, we use joint density-functional theory in tandem withsupporting electrochemical measurements to identify a novel theoretical pathwayfor the ORR on cubic Co3O4 nanoparticle electrocatalysts. This pathway alignsmore closely with experimental results than previous models. The new pathwayemploys the cracked adsorbates *(OH)(O) and *(OH)(OH), which, through hydrogenbonding, induce spectator surface *H. This results in an onset potentialclosely matching experimental values, in stark contrast to the traditional ORRpathway, which keeps adsorbates intact and overestimates the onset potential by0.7 V. Finally, we introduce electrochemical strain spectroscopy (ESS), agroundbreaking strain analysis technique. ESS combines ab initio calculationswith experimental measurements to validate proposed reaction pathways andpinpoint rate-limiting steps.

The Oxygen Reduction Pathway for Spinel Metal Oxides in Alkaline Media: An Experimentally Supported Ab Initio Study