Realizing Efficient Catalytic Performance and High Selectivity for Oxygen Reduction Reaction on a 2D Ni2SbTe2 Monolayer

One of the immediate challenges for the large-scale commercialization of hydrogen-based fuel cells is to develop cost-effective electrocatalysts to enable cathodic oxygen reduction reaction (ORR). Herein, we focus on the potential of the two-dimensional (2D) ternary chalcogenide Ni2SbTe2 monolayer as a high-performance electrocatalyst for the ORR using density function theory. Our computed results reveal that there are an obvious hybridization and electron transfer between the O 2p and Te 5p orbitals, which can activate the adsorbed oxygen and trigger the whole ORR process, with an overpotential as low as 0.33 V. In addition, the adsorption capacity of the monolayer surface for oxygen molecules can be effectively enhanced by doping with Fe or Co atoms. The Ni2SbTe2 monolayers doped with Fe or Co atoms not only maintain their original excellent ORR catalytic activity but also improve selectivity toward the four-electron (4e) reduction pathway. We highly anticipate that this work can provide excellent candidates and new ideas for designing low-cost and high-performance ORR catalysts to replace noble metal Pt-based catalysts in fuel cells.