High‐Entropy Zeolitic Imidazolate Frameworks for Dynamic Hydrogen Isotope Separation

Entropy-driven strategy enables the systematic design of complex systems by using entropy as a quantifiable design parameter for the degree of mixing. In this study, we present mixed-linker zeolitic imidazolate frameworks (ZIFs), sod-ZIF-1 series, that features two types of six-membered rings (6MRs) with aperture sizes of 3.4 Å and 1.7 Å. By adjusting the configurational entropy, the ratio of these 6MRs can be systematically controlled, which significantly influences adsorptive properties, particularly improving the H₂ affinity about 3 times throughout the series. This results in the significant enhancement of retention times in dynamic separation of hydrogen isotopes (D₂/H₂), even over LNG liquefaction temperature. This approach to entropy-driven pore engineering provides new opportunities for enhancing gas adsorption and separation processes.