High-throughput calculation-based rational design of Fe-doped MoS2 nanosheets for electrocatalytic pH-universal overall water splitting

Electrocatalytic water splitting is crucial for H2 generation via hydrogen evolution reaction (HER) but subject to the sluggish dynamics of oxygen evolution reaction (OER). In this work, single Fe atom-doped MoS2 nanosheets (SFe-DMNs) were prepared based on the high-throughput density functional theory (DFT) calculation screening. Due to the synergistic effect between Fe atom and MoS2 and optimized intermediate binding energy, the SFe-DMNs could deliver outstanding activity for both HER and OER. When assembled into a two-electrode electrolytic cell, the SFe-DMNs could achieve the current density of 50 mA cm−2 at a low cell voltage of 1.55 V under neutral condition. These results not only confirmed the effectiveness of high-throughput screening, but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.