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Double-atom catalysts provide a molecular platform for heterogeneous oxygen evolution electrocatalysis
Lichen Bai,+ Chia-Shuo Hsu,+ Duncan T.L. Alexander, Hao Ming Chen,* Xile Hu*
The oxygen evolution reaction (OER) is an essential anode reaction for the generation of fuels through water splitting or CO2 electroreduction. Mixed metal oxides containing Co, Fe or Ni have proved to be the most promising OER electrocatalysts in alkaline media. 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. Characterization reveals molecule-like bimetallic active sites for these supported catalysts. For each catalyst, we propose a catalytic cycle; all exhibit bimetallic cooperation and follow a similar O–O bond-forming step. 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.