Self‐Reconstructed Metal‐Organic Framework Heterojunction for Switchable Oxygen Evolution Reaction

Designing metal‐organic framework (MOF)‐based catalysts with superior oxygen evolution reaction (OER) activity and robust durability simultaneously is highly required yet very challenging due to the limited intrinsic activity and their elusive evolution under harsh OER conditions. Herein, a steady self‐reconstructed MOF heterojunction is constructed via redox electrochemistry and topology‐guided strategy. Thanks to the inhibiting effect from hydrogen bonds of Ni‐BDC‐1 (BDC=1,4‐benzenedicarboxylic acid), the obatained MOF heterojunction shows greatly improved OER activity with low overpotential of 225 mV at 10 mA cm−2, relative to the totally reconstructed Ni‐BDC‐3 (332 mV). Density function theory calculations reveal that the formed built‐in electric field in the MOF heterojunction remarkably optimizes the ad/desorption free energy of active Ni sites. Moreover, such MOF heterojunction shows superior durability attributed to the shielding effect of the surface‐evolved NiOOH coating. A self‐reconstructed metal‐organic framework (MOF) heterojunction is constructed via redox electrochemistry and topology‐guided strategy, and it exhibits superior oxygen evolution reaction (OER) activity and robust durability.