Zn‐Leaching Induced Rapid Self‐Reconstruction of NiFe‐Layered Double Hydroxides for Boosted Oxygen Evolution Reaction

Abstract Optimizing the active centers through reconstruction is recognized as the key to construct high‐performance oxygen evolution reaction (OER) catalysts. Herein, a simple and rapid in situ leaching strategy to promote the self‐reconstruction of NiFe‐layered double hydroxides (LDHs) catalysts is reported. The trace Zn dopants are introduced in advance by a facile and one‐step hydrothermal method, followed by leaching over the electrochemical activation process, which can remarkably reduce the formation potential of NiFeOOH active centers to enable the deeper self‐reconstruction for the formation of abundant highly active centers. Moreover, the self‐restructured NiFeOOH‐V Zn cannot only significantly lower the dehydrogenation energy barrier for the transformation from Ni(OH) 2 to NiOOH, but also decrease the free energy barrier of rate determining step for the *OH converted to *O through a deprotonation process, thus significantly boosting the OER behaviors. As a proof of concept, the obtained NiFeOOH‐V Zn catalyst just requires a low overpotential of 240 mV at 10 mA cm −2 , and delivers robust stability at 50 mA cm −2 over 120 h, which outperforms the benchmark of noble metal RuO 2 and those of most non‐noble metal catalysts ever reported.