Engineering Self‐Reconstruction via Flexible Components in Layered Double Hydroxides for Superior‐Evolving Performance

Abstract Most transition metal‐based catalysts for electrocatalytic oxygen evolution reaction (OER) undergo surface reconstruction to generate real active sites favorable for high OER performance. Herein, how to use self‐reconstruction as an efficient strategy to develop novel and robust OER catalysts by designing pre‐catalysts with flexible components susceptible to OER conditions is proposed. The NiFe‐based layered double hydroxides (LDHs) intercalated with resoluble molybdate (MoO 4 2− ) anions in interlayers are constructed and then demonstrated to achieve complete electrochemical self‐reconstruction (ECSR) into active NiFe‐oxyhydroxides (NiFeOOH) beneficial to alkaline OER. Various ex situ and in situ techniques are used to capture structural evolution process including fast dissolution of MoO 4 2− and deep reconstruction to NiFeOOH upon simultaneous hydroxyl invasion and electro‐oxidation. The obtained NiFeOOH exhibits an excellent OER performance with an overpotential of only 268 mV at 50 mA cm −1 and robust durability over 45 h, much superior to NiFe‐LDH and commercial IrO 2 benchmark. This work suggests that the ECSR engineering in component‐flexible precursors is a promising strategy to develop highly active OER catalysts for energy conversion.