Irreversible Conversion of a Water–Ethanol Solution into an Organized Two‐Dimensional Network of Alternating Supramolecular Units in a Hydrophobic Zeolite under Pressure

Turning disorder into organization is a key issue in science. By making use of X‐ray powder diffraction and modeling studies, we show herein that high pressures in combination with the shape and space constraints of the hydrophobic all‐silica zeolite ferrierite separate an ethanol–water liquid mixture into ethanol dimer wires and water tetramer squares. The confined supramolecular blocks alternate in a binary two‐dimensional (2D) architecture that remains stable upon complete pressure release. These results support the combined use of high pressures and porous networks as a viable strategy for driving the organization of molecules or nano‐objects towards complex, pre‐defined patterns relevant for the realization of novel functional nanocomposites.