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Metal–organic frameworks (MOFs) have introduced heterogeneity in their homogeneous matrix to create new functions that cannot be realized by each MOF individually. In this study, we chemically combined two different MOFs (UiO‐66 and HKUST‐1) in granola‐type granules (termed as HKUST‐1∧UiO‐66) to create a heterojunction of pores in nanocrystalline particles. The structure, morphology, elemental composition, and pore environment were characterized to confirm that two types of pores are in conjunction all over the HKUST‐1∧UiO‐66 granules. We found that the HKUST‐1∧UiO‐66 granules showed an enhanced CO2sorption capacity than its constituents due to the complexity and the heterojunction of pores inside. Moreover, the HKUST‐1∧UiO‐66 granules present four and two times higher formaldehyde removal capacity than those of the HKUST‐1 and UiO‐66 samples, respectively. The nanocrystalline HKUST‐1 was granulized with UiO‐66 to obtain a heterojunction of pores in granola‐type granules, which enhances capacities for carbon dioxide uptake at low temperature and formaldehyde removal in ambient temperature and pressure.

Deuterium has been recognized as an irreplaceable element in industrial and scientific research. However, hydrogen isotope separation still remains a huge challenge due to the identical physicochemical properties of the isotopes. In this paper, a partially fluorinated metal–organic framework (MOF) with copper, a so-called FMOFCu, was investigated to determine the separation efficiency and capacity of the framework for deuterium extraction from a hydrogen isotope mixture. The unique structure of this porous material consists of a trimodal pore system with large tubular cavities connected through a smaller cavity with bottleneck apertures with a size of 3.6 Å plus a third hidden cavity connected by an even smaller aperture of 2.5 Å. Depending on the temperature, these two apertures show a gate-opening effect and the cavities get successively accessible for hydrogen with increasing temperature. Thermal desorption spectroscopy (TDS) measurements indicate that the locally flexible MOF can separate D2from anisotope mixture efficiently, with a selectivity of 14 at 25 K and 4 at 77 K.