Multilayered Molybdate Microflowers Fabricated by One‐Pot Reaction for Efficient Water Splitting

The development of high‐performance, low‐cost and rapid‐production bifunctional electrocatalysts towards overall water splitting still poses huge challenges. Herein, the authors utilize a facile hydrothermal method to synthesize a novel structure of Co‐doped ammonium lanthanum molybdate on Ni foams (Co‐ALMO@NF) as self‐supported electrocatalysts. Owing to large active surfaces, lattice defect and conductive channel for rapid charge transport, Co‐ALMO@NF exhibits good electrocatalytic performances which requires only 349/341 mV to achieve a high current density of 600 mA cm(−2) for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Besides, a low cell voltage of 1.52 V is required to reach the current density of 10 mA cm(−2) in alkaline medium along with an excellent long‐term stability for two‐electrode configurations. Density functional theory calculations are performed to reveal the reaction mechanism on Co‐ALMO@NF, which shows that the Mo site is the most favorable ones for HER, while the introduction of Co is beneficial to reduce the adsorption intensity on the surface of Co‐ALMO@NF, thus accelerating OER process. This work highlighted the importance of the structural design for self‐supporting electrocatalysts.