Double-Atom Catalysts Provide a Molecular Platform for Oxygen Evolution

17 December 2019, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

The oxygen evolution reaction (OER) is an essential anode reaction for the generation of solar and electric fuels through water splitting or CO2 electroreduction. Mixed metal oxides containing Co, Fe, or Ni prove to be the most promising OER electrocatalysts in alkaline medium. However, the active sites and reaction mechanisms of these catalysts are difficult to study due to their heterogeneous nature. Here we describe a general synthesis of Co, Fe, and Ni-containing double-atom catalysts from their single-atom precursors via in-situ electrochemical transformation. Atomic-resolution microscopy and operando X-ray absorption spectroscopy (XAS) reveal molecule-like bimetallic active sites for these supported catalysts. Based on electrokinetic and XAS data, we propose a complete catalytic cycle for each catalyst. These mechanisms follow a similar O-O bond forming step and all exhibit bimetallic cooperation. However, the mechanisms diverge in the site and source of OH- for O-O bond formation as well as the order of proton and electron transfer. Our work demonstrates double-atom catalysts as an attractive platform for fundamental studies of heterogeneous OER electrocatalysts.

Keywords

Oxygen Evolution Reaction
electrocatalysis
double-atom catalysts
mechanism
electrokinetics

Supplementary materials

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