Alkali co-adsorption enhances bond-resolved N2 activation at O2-active MoS2 single-atom sites

This dataset supports a spin-polarized density functional theory study examining whether O₂-activation-favorable active-site environments at Fe- and Co-substituted sulfur vacancies in monolayer MoS₂ can produce a comparable response for H-free N₂ adsorption. Side-on and end-on N₂ adsorption branches were evaluated together with projected density of states and crystal orbital Hamilton population analyses to distinguish coordination geometry, thermodynamic preference, and intramolecular bond weakening. A perpendicular electric field and K/Na co-adsorption were further considered as physical and chemical perturbations. The calculations show that shared side-on coordination does not produce O₂-like N₂ activation, while the thermodynamically preferred end-on branch retains a shorter and stronger N–N bond. Alkali co-adsorption substantially enhances N–N bond weakening but does not eliminate the O₂–N₂ activation gap or reverse the end-on thermodynamic preference. The archive provides the optimized structures, representative computational input and output data, and numerical source data supporting the reported analyses.