Building intercalation structure for high ionic conductivity via aliovalent substitution

Two-dimensional (2D) materials, which possess robust nanochannels, high flux and allow scalable fabrication, provide new platforms for nanofluids. Highly efficient ionic conductivity can facilitate the application of nanofluidic devices for modern energy conversion and ionic sieving. Herein, we propose a novel strategy of building an intercalation crystal structure with negative surface charge and mobile interlamellar ions via aliovalent substitution to boost ionic conductivity. The Li_2xM_1-xPS₃ (M = Cd, Ni, Fe) crystals obtained by the solid-state reaction exhibit distinct capability of water absorption and apparant variation of interlayer spacing (from 0.67 to 1.20 nm). The assembled membranes show the ultrahigh ionic conductivity of 1.20 S/cm for Li_0.5Cd_0.75PS₃ and 1.01 S/cm for Li_0.6Ni_0.7PS₃. This facile strategy may inspire the research in other 2D materials with higher ionic transport performance for nanofluids.