The rational design of oxygen evolution reaction (OER) catalysts from the perspective of electronic structure is highly desirable to optimize electrocatalytic activity. Monometallic phosphides such as Ni 2 P have been shown to be active toward OER, but their performance remains unsatisfactory. Herein, guided by the theoretical mechanism study of the intrinsic high electroactivity revealed in the d-band center (E d ) theory, the Fe-substituted Ni 2 P ((Ni x Fe 1−x ) 2 P) nanosheets grown directly on NiFe foam are designed and synthesized. As OER electrocatalysts in alkaline media, the (Ni x Fe 1−x ) 2 P nanosheets show an overpotential of 166 mV to deliver the current density of 10 mA cm −2 , which is superior to the Ni 2 P and most reported transition-metal-based catalysts. Combining DFT simulations with experiments reveals that the enhanced activity results from the moderate rise in E d energy levels, which balances the adsorption and desorption capacities of the oxygen-containing intermediates (*O, *OH, and *OOH). This work supplies valuable insights for the rational design and construction of efficient doped electrocatalysts under the guidance of the d-band center theory.
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