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(H 2 O) 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 (MoS 2 ) superlattice nanoflower (1T‐MoS 2 ‐NC) and Na(H 2 O) 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(H 2 O) 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‐MoS 2 ‐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.