Sulfur and oxygen dual vacancies manipulation on 2D NiS2/CeO2 hybrid heterostructure to boost overall water splitting activity

It is still an enormous challenge to develop non-precious electrocatalysts through low-cost and efficient methods. To fulfill highly active site exposure and optimized intrinsic activity, the 2-dimensional NiS2/CeO2 with unique heterostructure and abundant sulfur and oxygen vacancies (v-NiS2/CeO2 HS) was prepared by solvothermal reaction and annealing. The density functional theory calculations illustrate that the materials with both heterostructure and vacancies simultaneously have a positive effect on promoting the kinetics of oxygen evolution reaction and hydrogen evolution reaction and optimizing the adsorption energy of hydrogen. As a result, v-NiS2/CeO2 HSs deliver the current density of 10 mA/cm2 at the low overpotential of 271 mV for oxygen evolution reaction and the overpotential required by v-NiS2/CeO2 HSs for hydrogen evolution reaction is 123 mV (at 10 mA/cm2). The v-NiS2/CeO2 HSs demand a lower cell voltage with 1.64 V (at 10 mA/cm2) toward overall water splitting. These results provide a theoretical and practical direction for the development of low-cost, earth-abundant electrocatalysts. •The 2-dimensional (2D) NiS2/CeO2 heterostructures (HSs) contain abundant sulfur and oxygen vacancy.•The 2D NiS2/CeO2 HSs possess unique 2D heterostructures.•Density functional theory demonstrated that the vacancy and heterostructure synergistically accelerate the reaction kinetics for hydrogen evolution reaction and oxygen evolution reaction.•The 2D NiS2/CeO2 HSs have significantly enhanced performance of water splitting performance.