Dopant-enhanced sodium and potassium-ion adsorption and diffusion in two-dimensional titanium disulfide

Two-dimensional (2D) titanium disulfide (TiS[Formula: see text]) is the lightest transition-metal dichalcogenide (TMD). It exhibits relatively better adsorption and diffusion of sodium (Na) and potassium (K) ions than other TMDs, such as MoS[Formula: see text] (molybdenum disulfide) and ReS[Formula: see text] (rhenium disulfide), making it a promising anode material for alkali-ion batteries. Previous studies have found that doping significantly enhances the adsorption and diffusion capabilities of 2D TMDs. For the first time, this work reports the adsorption of Na and K ions on doped TiS[Formula: see text] monolayers using first-principles calculations, where the Ti atom is substituted by 3d-transition metals, including iron (Fe), cobalt (Co), nickel (Ni), and copper (Cu). Metal-atom doping induces remarkably stronger binding of alkali ions on the surface of TiS[Formula: see text], with adsorption energies ranging from [Formula: see text]2.07 to [Formula: see text]2.48 eV for Na and [Formula: see text]2.59 to [Formula: see text]3.00 eV for K. The diffusion barrier energies for alkali ions decrease in the proximity of the doping site and increase as the ions travel away from the doping site for Fe-, Co-, and Ni-doped TiS[Formula: see text]. The average open circuit voltage increases dramatically when Na ions are adsorbed on Fe-doped TiS[Formula: see text] (by 62%) and Co-doped TiS[Formula: see text] (by 61%), while K ions result in a moderate improvement of 9% and 8%, respectively. These findings suggest that metal-atom doping considerably improves the electrochemical properties of 2D TiS[Formula: see text], potentially enabling its use as anode materials in Na- and K-ion batteries.