Rational engineering of metal–organic coordination networks into facet‐controlled phosphides for overall water splitting

Abstract Although transition metal phosphide electrocatalysts display unique electronic structure that serves as functional centers for hydrogen evolution reaction, the synthesis of this class materials oxygen remains a challenge due to complex multielectron transfer pathways and sluggish reaction kinetics. This study details an in‐situ modification transformation cyanide‐bridged nickel‐iron (CN‐NiFe) organometallic hybrid into preferential Fe 2 P phase with prevailing exposed faceted active by leveraging on facile coordinate cleavage dynamics compound reactivity labile organic coordination frameworks. The resultant attains high electrochemical surface area, low Tafel slope, overpotential while also demonstrating bifunctional electrocatalytic performance overall water splitting. Comprehensive experimental studies density theory calculations reveal exceptional catalytic activity originates from framework metallic sites allows optimal adsorption intermediates. image