NiN3-Embedded MoS2 Monolayer as a Promising Electrocatalyst with High Activity for Oxygen Evolution Reaction: A Computational Study

Electrocatalytic oxygen evolution reaction (OER) plays a crucial role on the conversion of the renewable electricity into storable fuels, in which the development of stable, low-cost, and efficient catalysts is highly crucial to boost the sluggish kinetics of OER for achieving high efficiency. In this work, by means of comprehensive density functional theory (DFT) computations, we proposed a new class of OER catalyst, i.e., TMN3@MoS2, in which several TMN3 moieties was embedded into MoS2 monolayer. Our results revealed that the introduction of N dopants can greatly enhance the binding strength between TM atoms and MoS2 monolayer, thus rendering them excellent stability, which was further verified by the ab-initio molecular dynamics simulations, dissolution potential, and diffusion barrier. In particular, according to the computed free energy changes, the NiN3@MoS2 was revealed to exhibit the best OER catalytic activity due to its ultralow overpotential of 0.45 V for OER. Interestingly, multiple-level descriptors, including ΔGO*-ΔGOH*, d-band center, and φ involving the local structural and chemical environment of the reaction site can well rationalize the origin of the high catalytic activity of NiN3@MoS2 for the OER. Our findings not only open a new avenue to design OER catalysts with high stability, superior activity, and low cost, but also offer promising descriptors to accelerate the screening of OER catalysts as the alternatives of the well-established noble Ru/Ir-based catalysts.