We report the synthesis of nitridation-induced NiFe-MOF through post-synthetic functionalization of terminal ligand in NiFe-MOF nanosheet. We directly identify the key factor of amino ligand in N-NiFe-MOF for boosting the OER performance through combining single X-ray crystallographic characterization and in-situ Raman tracking, as well as ex-situ spectroscopy analysis. Density functional theory (DFT) calculations and experimental results indicate irreversible phase reconstruction from amino ligand oxidation prior to OER could lead to the optimized ΔG_*O, resulting in the remarkable OER performance with an overpotential of 258 mV to obtain the current density of 100 mA cm⁻² in 1.0 M KOH solution. Our work will provide new strategy for rational designing advanced MOF-based OER electrocatalysts.

https://doi.org/10.1016/j.jechem.2021.05.024