Synergistic effects of Fe and P doping in WS₂ monolayers for enhanced bifunctional electrocatalysis in water splitting

The quest for efficient dual-purpose electrocatalysts to facilitate water splitting is an ongoing challenge in materials science. In this study, we introduce a novel approach involving the incorporation of Fe and P atoms into WS₂ monolayers (MLs) through rigorous first-principle calculations. The introduction of Fe and P atoms brings about remarkable enhancements in the electronic properties of the WS₂ MLs, significantly boosting the catalytic performance of the 1T’ phase. The doping-induced changes in energy levels lead to the formation of a spin-polarized density of states, which exhibits superior conductivity in the vicinity of the d-band center and Fermi level. These electronic alterations are intricately governed by the valence and conduction bands. In addition to this, the introduced dopants elevate the charge transfer rate while simultaneously reducing interfacial resistance. Furthermore, the strong bonding of the dopants plays a pivotal role in reducing the energy barrier during adsorption. This, in turn, leads to a substantial decrease in the Gibbs free energy (0.101 eV) for the hydrogen evolution reaction and a lowered overpotential (0.36 V) for the oxygen evolution reaction. These findings collectively offer a promising avenue for the development of advanced bifunctional catalysts in the context of water splitting, suggesting that substitutional heteroatom doping of 1T′-WS₂ MLs holds substantial potential in this field.