Hydration of methane intercalated in Na-smectites with distinct layer charge: Insights from molecular simulations

► Interlayer CH4 can be solvated by 12-13 water molecules and coordinated with 5-6 oxygen atoms from the clay surface. ► Tetrahedral negative charge makes for CH4 hydration in smectite. ► Stability of the interlayer CH4 hydrate follows the order of SWy < SAz < NAu.