Synergistically integrated Co₉S₈@NiFe-layered double hydroxide core-branch hierarchical architectures as efficient...

Efficient, low-cost, and robust electrocatalysts development for overall water splitting is highly desirable for renewable energy production yet still remains challenging. In this work, Co₉S₈ nanoneedles arrays are synergistically integrated with NiFe-layered double hydroxide (NiFe-LDH) nanosheets to form Co₉S₈@NiFe-LDH core-branch hierarchical architectures supported on nickel foam (Co₉S₈@NiFe-LDH HAs/NF). The Co₉S₈@NiFe-LDH HAs/NF exhibits high catalytic performances for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) with overpotential of 190 and 145 mV at 10 mA cm^-2, respectively. The density functional theory calculations predict that the synergy between Co₉S₈ and NiFe-LDH contributes to the high catalytic performance by lowering the energy barrier of HER. When used as both anode and cathode electrocatalyst, it can deliver 10 mA cm^-2 at a low cell voltage of 1.585 V with excellent long-term durability. This work opens a new avenue toward the exploration of highly efficient and stable electrocatalyst for overall water splitting.