Lattice contraction-driven design of highly efficient and stable O–NiFe layered double hydroxide electrocatalysts for water oxidation

Abstract

The slow progress of the oxygen evolution reaction (OER) is a key challenge in advancing water splitting as a viable technology for sustainable hydrogen production. Utilizing a self-standing NiFe layered double hydroxide (LDH) is a promising approach to address the slow kinetics of OER. Herein, the oxidized Fe2+-containing NiFe-LDH supported on Ni foam (O–NiFe-LDH@NF) is developed through corrosion engineering and aging. The growth mechanism is studied by adjusting urea content, hydrothermal temperature and time. It is revealed that the transformation of Fe2+ to Fe3+ in Fe2+-containing NiFe-LDH and the increase of Fe content leads to lattice contraction. Furthermore, detailed experiments and theoretical simulations illustrate that the substantial Fe content and lattice shrinkage promote the generation of Ni in high oxidation state and enhance the adsorption affinity toward the reaction species. Consequently, O–NiFe-LDH@NF exhibits enhanced OER activity and stability, with an exceptionally low overpotential of 197 mV and 354 mV observed at the current densities of 10 and 500 mA cm−2, respectively, and remarkable stability over 300 h. This approach can be generalized for designing advanced electrocatalysts.