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Membrane‐based separation has the merit of low carbon footprint. In this study, the pore size of metal–organic framework (MOF) membranes is rationally designed for discriminating various pairs of hydrocarbon isomers. Specifically, Zr‐MOF UiO‐66 (UiO stands for University of Oslo) membranes are developed for separating p/o‐xylene due to their proper pore size. For n‐hexane/2‐methylpentane separation,...