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Abstract Oxygen evolution reaction (OER) over perovskite oxides, upon undergoing a lattice oxygen oxidation mechanism, is strongly oxygen vacancy‐correlated as determined by the oxygen ion diffusivity. Despite substantial efforts having been devoted to tuning the oxygen vacancy concentration in perovskite oxides, the impact of the concomitant altering of oxygen vacancy ordering is often underestimated. In particular, the underlying mechanism of how the ordering and the concentration of oxygen vacancy affect the lattice OER, and how to well balance them still remain inadequately understood. Herein, a series of Sr 1− x Ca x Co 0.5 Fe 0.5 O 3− δ with gradually increased oxygen vacancy concentration and ordering are synthesized. Theoretical calculations indicated that a higher oxygen vacancy concentration promoted the lattice oxygen migration, whereas a higher oxygen vacancy ordering impeded it. Particularly, Sr 0.5 Ca 0.5 Co 0.5 Fe 0.5 O 3− δ with a relatively higher oxygen vacancy concentration and a lower ordering displayed the maximum oxygen diffusion rate and the optimal OER activity, affording a current density of 10 mA cm −2 at a quite low overpotential of 310.2 mV, together with a small Tafel slope of 55.87 mV dec −1 . This study sheds light on the critical influence of oxygen vacancy configuration on the lattice OER, and paves a compromised avenue to screen and design advanced electrocatalysts for various electrochemical devices.
Liu et al. (Thu,) studied this question.