Molecular Intercalation and Electron Modulation Stabilized 1T-MoS2 Superlattice Nanoflowers with Desolvation Regulation for Energy-Efficient Water Production

Abstract

The desolvation of hydrated sodium ions (Na(H₂O)_x⁺) at the electrode/electrolyte interface is crucial for aqueous sodium-storage systems, but the rational regulation of desolvation process remains a significant challenge. Herein, a dual structural engineering strategies of electron configuration modulation and molecular intercalation for the regulation of desolvation kinetics between nitrogen-doped lamellar carbon-intercalated 1T-molybdenum disulfide (MoS₂) superlattice nanoflower (1T-MoS₂-NC) and Na(H₂O)_x⁺ is demonstrated. The synergy of cation-π interaction and adjustable interlayer structure induced by NC intercalation reduces the desolvation energy and promotes dehydration degree of Na(H₂O)_x⁺, thereby providing more interspace for Na⁺ accommodation. The abundant 1T metal phase accelerates the charge transfer while lowering the Na⁺ diffusion energy barrier. Benefitting from the advantages above, 1T-MoS₂-NC exhibits superior capacitive deionization performance, including outstanding brackish water desalination capacity (80.9 mg_NaCl g⁻¹) and splendid long-term stability in a 1000 mg L⁻¹ NaCl solution at a cell voltage of 1.4 V, which exceeds most of the state-of-the-art electrodes under similar experimental conditions. This finding reveals the facilitating effect of desolvation regulation on sodium-ion storage, paving the way for advanced electrochemical aqueous ion storage applications.