Engineering Lattice Oxygen Regeneration of NiFe Layered Double Hydroxide Enhances Oxygen Evolution Catalysis Durability

The lattice oxygen mechanism (LOM) endows NiFe layered double hydroxide (NiFe‐LDH) with superior oxygen evolution reaction (OER) activity, yet the frequent evolution and sluggish regeneration of lattice oxygen intensify the dissolution of active species. Herein, we overcome this challenge by constructing the NiFe hydroxide/Ni4Mo alloy (NiFe‐LDH/Ni4Mo) heterojunction electrocatalyst, featuring the Ni4Mo alloy as the oxygen pump to provide oxygenous intermediates and electrons for NiFe‐LDH. The released lattice oxygen can be timely offset by the oxygenous species during the LOM process, balancing the regeneration of lattice oxygen and assuring the enhancement of the durability. In consequence, the durability of NiFe‐LDH is significantly enhanced after the modification of Ni4Mo with an impressively durability for over 60 h, much longer than that of NiFe‐LDH counterpart with only 10 h. In‐situ spectra and first‐principle simulations reveal that the adsorption of OH− is significantly strengthened owing to the introduction of Ni4Mo, ensuring the rapid regeneration of lattice oxygen. Moreover, NiFe‐LDH/Ni4Mo‐based anion exchange membrane water electrolyzer (AEMWE) presents an impressive durability for over 150 h at 100 mA cm−2. The oxygen pump strategy opens opportunities to balance the evolution and regeneration of lattice oxygen, enhancing the durability of efficient OER catalysts.