Solvated-Electron-Driven Intercalation Enables Electron-Rich K_xNbS₂ Construction and Exfoliation

While creating electron-rich states can tune material properties, achieving this in van der Waals (vdW) materials lacking cationic frameworks remains challenging. Here, we report a molten-salt solvated-electron strategy that injects electrons into the vdW gaps of transition metal dichalcogenides (TMDCs). Using a Ga-KCl system, we construct an electron-rich intermediate K_xNbS₂ (x≤0.5), wherein coupled K⁺ intercalation provides charge compensation and drives superlattice formation. Spectroscopic characterization confirm electron injection and partial reduction of the host lattice. This state enables solvent-dependent exfoliation, protic solvents drive a chemical pathway, whereas aprotic solvents facilitate physical delamination via electrostatic repulsion. Demonstrating applicability across TMDCs (NbS₂, TaS₂, NbSe₂ and WS₂), alkali salts, and electron donors, this strategy provides a route to engineer the electronic structures and interlayer interactions of two-dimensional (2D) materials for catalysis and quantum applications.