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Core-shell ZIF-8@ZIF-67- and ZIF-67@ZIF-8-based zeolitic imidazolate frameworks (ZIFs) were synthesized solvothermally using a seed-mediated methodology. Transmission electron microscopy-energy-dispersive X-ray spectrometry, line scan, elemental mapping, X-ray photoelectron spectroscopy, and inductively coupled plasma-atomic emission spectroscopy analyses were performed to confirm the formation of a core-shell structure with the controlled Co/Zn elemental composition of ∼0.50 for both the core-shell ZIFs. The synthesized core-shell ZIF-8@ZIF-67 and ZIF-67@ZIF-8 frameworks conferred enhanced H 2 (2.03 and 1.69 wt %) storage properties at 77 K and 1 bar, which are ca. 41 and 18%, respectively, higher than that of the parent ZIF-8. Notably, the distinctly remarkable H 2 storage properties shown by both the core-shell ZIFs over the bimetallic Co/Zn-ZIF and the physical mixture of ZIF-8 and ZIF-67 clearly evidenced their unique structural properties (confinement of porosity) and elemental heterogeneity due to the core-shell morphology of the outperforming core-shell ZIFs. Moreover, H 2 adsorption isotherm data of these frameworks are best fitted with the Langmuir model ( R  2 ≥ 0.9999). Along with the remarkably enhanced H 2 storage capacities, the core-shell ZIFs also displayed an improved CO 2 capture behavior. Hence, we demonstrated here that the controlled structural features endorsed by the rationally designed porous materials may find high potential in H 2 storage applications.

Core–Shell Zeolitic Imidazolate Frameworks for Enhanced Hydrogen Storage