Plasma-Tailored Heterostructured Ni-Ni3N Nanosheets for Enhanced Overall Water Splitting

Heterostructured frameworks have received considerable research interest because of the superior integrity of different components and hence favorable electrocatalytic behavior. Currently, Ni-Ni 3 N-based heterostructures are regarded as one of the most essential candidates for electrocatalytic water splitting. However, most reported heterostructures were achieved based on a thermal technique, leading to restricted heterostructured components for electrochemical behavior. Here, we have provided a facile plasma strategy to modulate hierarchical Ni-Ni 3 N nanostructures (hNiN) for optimized water splitting. By controlling the plasma processing duration, hNiN-based nano-frameworks have delivered maximized activity in hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The hNiN-300 can deliver a potential of 150 mV with the current of 10 mA cm −2 ( η 10 ) of HER, while the hNiN-30 exhibits the best OER catalytic activity with the current density of 167 mV at 10 mA cm −2 ( η 10 ). Also, the hNiN have excellent cyclic performances with little activity degradation after cycling. Based on experimental characterizations and computational analysis, the good water splitting behavior of hNiN can be attributed to the heterostructural formation between Ni 3 N and Ni. Such work can provide a novel pathway to easily modulate nitride-based heterostructures for superior electrochemical water splitting. Graphical Abstract Plasma strategy can easily modulate hierarchical Ni-Ni 3 N heterostructures for optimized electrocatalytic water splitting.