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Tuning the reactivity of lattice oxygen is of significance for lowering the energy barriers and accelerating the oxygen evolution reaction (OER). Herein, single-atomic Mo sites are anchored on Ni-Fe oxyhydroxide nanoarrays by a facile metal-organic-framework-derived strategy, exhibiting superior performance toward the OER in alkaline media. In situ electrochemical spectroscopy and isotope-labeling experiments reveal the involvement of lattice oxygen during OER cycles. Combining theoretical and experimental investigations of the electronic configuration, it is comprehensively confirmed that the incorporation of single-atomic Mo sites enables higher oxidation state of the metal and strengthened metal-oxygen hybridization, as well as the formation of oxidized ligand holes above the Fermi level. In a word, the considerable acceleration of water oxidation is achieved via enhancing the reactivity of lattice oxygen and triggering the lattice oxygen activation. This work may provide new insights for designing ideal electrocatalysts via tuning the chemical state and activating the anions ligands.
Wu et al. (Mon,) studied this question.