Organic-inorganic superlattices are a class of artificial structures of significant scientific and technological importance. Forming these hybrid materials can be achieved via controlled intercalation of organic molecules into inorganic layered hosts, which is a complex course involving multiple physicochemical processes. In solution phase, it is further complicated by interaction of solvent molecules with the intercalant and/or host. Here we describe an intercalation system exhibiting strong solvent-dependent kinetics and phase evolution. In revisiting intercalation of ferrocene into layered VOPO4·2H2O material by taking into account the influence of solvent, we are able to unravel molecular configurations of ferrocene molecules. An exclusive orientation of ferrocene but different arrangements among the layers are concluded in two model solvents. Resolving this complicated structure is possible thanks to a combined experimental and theoretical approach. Our study provides new insights into understanding molecular configurations and controlling intercalation kinetics in creating organic-inorganic superlattices, which may offer unprecedented properties beyond conventional materials.
Keywords: Solvent effect; intercalation; layered crystal; metallocene; organic−inorganic superlattice.