Water splitting is an environmentally friendly strategy to produce hydrogen but is limited by the oxygen evolution reaction (OER). Therefore, there is an urgent need to develop highly efficient electrocatalysts. Here, NiFe layered double hydroxides (NiFe LDH) with tunable Ni/Fe composition exhibit corresponding dependent morphology, layered structure, and chemical states, leading to higher activity and better stability than that of conventional NiFe LDH-based catalysts. The characterization data show that the low overpotentials (249 mV at 10 mA cm -2 ), ultrasmall Tafel slopes (24 mV dec -1 ), and high current densities of Ni 3 Fe LDH result from the larger fraction of trivalent Fe 3+ and the optimized local chemical environment with more oxygen coordination and ordered atomic structure for the metal site. Owing to the active intermediate species, Ni(Fe)OOH, under OER conditions and a reversible dynamic phase transition during the cycling process, the Ni 3 Fe LDH achieves a high current density of over 2 A cm -2 at 2.0 V, and durability of 400 h at 1 A cm -2 in a single cell test. This work provides insights into the relationship between the composition, electronic structure of the layer, and electrocatalytic performance, and offers a scalable and efficient strategy for developing promising catalysts to support the development of the future hydrogen economy.

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Although the effect of magnetic field (B) on electrochemical reactions (magnetoelectrolysis phenomenon) has been long known, it has not been considered in electrochemical reactions analyzed in situ by magnetic resonance methods, such as nuclear magnetic resonance (NMR), electron paramagnetic resonance (EPR), and magnetic resonance imaging (MRI), which are intrinsically performed in the presence of B. In this report, the effect of B on the copper electrodeposition reaction, measured by a low-field (0.23 T) NMR spectrometer, was demonstrated. As expected, an enhancement in the reaction rate in comparison to the ex situ electrodeposition reaction was observed. Such enhancement was not dependent on electrodes/magnetic field orientations. Parallel and perpendicular orientations showed similar electrodeposition rates, which is explained by the cyclotron flows generated by distortions in electric and magnetic field lines near the electrode and the electrode edge. Therefore, NMR spectroscopy is not a passive analytical method, as assumed in preceding in situ spectroelectrochemical studies. Although the magnetoelectrolysis phenomenon demonstrated in this report used a paramagnetic ion, it can also be observed for diamagnetic species, since the magnetoelectrolysis phenomenon is independent of the nature of the species. Consequently, similar convection effects may occur in other electrochemical nuclear magnetic resonance (EC-NMR) experiments, such as the electrochemical reaction of organic molecules, as well as in electrocatalysis/fuel cells, lithium-ion batteries, and experiments that use electrochemical electron paramagnetic resonance (EC-EPR) and electrochemical magnetic resonance imaging (EC-MRI).

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