Double-atom catalysts as a molecular platform for heterogeneous oxygen evolution electrocatalysis

Lichen Bai, Chia-Shuo Hsu, Duncan T. L. Alexander, Hao Ming Chen () and Xile Hu ()
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Lichen Bai: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL), EPFL-ISIC-LSCI, BCH 3305
Chia-Shuo Hsu: National Taiwan University
Duncan T. L. Alexander: Interdisciplinary Centre for Electron Microscopy (CIME), Ecole Polytechnique Fédérale de Lausanne (EPFL)
Hao Ming Chen: National Taiwan University
Xile Hu: Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL), EPFL-ISIC-LSCI, BCH 3305

Nature Energy, 2021, vol. 6, issue 11, 1054-1066

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41560-021-00925-3

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