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Abstract The oxygen evolution reaction (OER) activity of single‐atom catalysts (SACs) is closely related to the coordination environment of the active site. Oxygen‐coordinated atomic metal species bring about unique features beyond nitrogen‐coordinated atomic metal species due to the fact that the M–O bond is weaker than the M–N bond. Herein, a series of metal–oxygen–carbon structured low‐nucleus clusters (LNCs) are successfully anchored on the surface of multiwalled carbon nanotubes (M‐MWCNTs, M = Ni, Co, or Fe) through a foolproof low‐temperature gas transfer (300°C) method without any further treatment. The morphology and coordination configuration of the LNCs at the atomic level were confirmed by comprehensive characterizations. The synthetic Ni‐MWCNTs electrocatalyst features excellent OER activity and stability under alkaline conditions, transcending the performances of Co‐MWCNTs, Fe‐MWCNTs and RuO 2 . Density functional theory calculations reveal that the moderate oxidation of low‐nucleus Ni clusters changes the unoccupied orbital of Ni atoms, thereby lowering the energy barrier of the OER rate‐limiting step and making the OER process more energy‐efficient. This study demonstrates a novel versatile platform for large‐scale manufacturing of oxygen‐coordinated LNC catalysts.
Ji et al. (Mon,) studied this question.