Abstract
Rational design of non-precious metal catalysts can accelerate the oxygen evolution reaction (OER) kinetics. Herein, inspired by theoretical analysis, in-situ Fe-doped Ni2P/Ni12P5 with rich P vacancies (Fe-NiPx) is designed and constructed, in which the production of P vacancies is induced by Fe doping. Relevant characterizations confirm that the Fe doping and P vacancies can co-adjust the crystal and electronic structures, thereby optimizing the reconstruction behavior and improving the intrinsic activity of reconstructed-derived Ni(Fe)OOH. As a result, it exhibits excellent OER activity with overpotentials of 256 and 276 mV to achieve the current density of 100 mA cm−2 in 1 M KOH solutions and alkaline seawater, respectively. Furthermore, the Fe-NiPx electrode only requires 1.861 and 1.889 V to drive the 1.0 A cm−2 overall water and seawater splitting, respectively, and maintains stable output as high as 1000 h. Also, to demonstrate the great application potential, green energy-to-hydrogen systems are established. Electrochemical tests and theoretical calculations reveal that reconstructed-Fe-NiPx facilitates the OER kinetics under the adsorbate evolution mechanism (AEM) pathway, with optimized adsorption free energies of intermediates and reduced reaction energy barriers. This work provides new insights into efficient water and seawater splitting through in-situ heteroatom doping and vacancy engineering.
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