Computational Screening for High-Activity MoS2 Monolayers-Based Catalysts for the Oxygen Reduction Reaction via Substitutional Doping with Transition Metal
Rational design of non-noble materials as highly efficient, economical, and durable platinum-free oxygen reduction reactions (ORR) electrocatalysts is crucial to the large-scale application of fuel cells. In this work, by means of density functional theory (DFT) computations, we have systemically explored the catalytic activity of the substitutionally doped MoS2 monolayers with various transition metals (TM) atoms for the ORR. Our computations reveal that these TM atoms can strongly interact with the S-vacancy and significantly modify the electronic and magnetic properties of MoS2 monolayer. On the basis of the computed free energies, it is evident that Cu-embedded MoS2 monolayer exhibits the best ORR catalytic activity with the minimum overpotential of 0.63 V due to its optimal interaction with ORR species. Thus, our study suggests that the substituted doping with suitable transition metal is expected be an effective method to improve the catalytic activity of MoS2 monolayer for the ORR, which could provide a useful guidance for the development of novel 2D ORR electrocatalysts.