In this article, the effect of a porous material’s flexibility on the dynamic reversibility of a nonwetting liquid intrusion was explored experimentally. For this purpose, high-pressure water intrusion together with high-pressure in situ small-angle neutron scattering were applied for superhydrophobic grafted silica and two metal–organic frameworks (MOFs) with different flexibility [ZIF-8 and Cu2(tebpz) (tebpz = 3,3′,5,5′tetraethyl-4,4′-bipyrazolate)]. These results established the relation between the pressurization rate, water intrusion–extrusion hysteresis, and porous materials’ flexibility. It was demonstrated that the dynamic hysteresis of water intrusion into superhydrophobic nanopores can be controlled by the flexibility of a porous material. This opens a new area of applications for flexible MOFs, namely, a smart pressure-transmitting fluid, capable of dissipating undesired vibrations depending on their frequency. Finally, nanotriboelectric experiments were conducted and the results showed that a porous material’s topology is important for electricity generation while not affecting the dynamic hysteresis at any speed.

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Gas separation performances are usually degraded under humid conditions for many crystalline porous materials because of the lack of water stability and/or the competition of water vapor toward the interaction sites (e.g., open metal sites). Zeolitic imidazolate frameworks (ZIFs) are suitable candidates for practical applications in gas separation because of their excellent physical/chemical stabilities. However, the limitation of substituent positions in common ZIFs has prevented extensive pore engineering to improve their separation performance. In a type of gyroidal ZIFs with gie topology, the Schiff base moiety provides additional substituent positions, making it possible to modify the spatial arrangement of hydrophobic methyl groups. Herein, a new gyroidal ZIF, ZnBAIm (H2BAIm = 1,2-bis­(1-(1H-imidazol-4-yl)­ethylidene)­hydrazine), is designed, synthesized, and characterized. The spatially modified ZnBAIm exhibits improved thermal/chemical/mechanical stabilities compared to ZnBIm (H2BIm = 1,2-bis­((5H-imidazol-4-yl)­methylene)­hydrazine). ZnBAIm can remain intact up to about 480 °C in a N2 atmosphere and tolerate harsh treatments (e.g., 5 M NaOH aqueous solution at room temperature for 24 h and 190 MPa high pressure in the presence of water). Moreover, the modified pore and window sizes have improved significantly the ethane/ethylene selectivity and separation performance under humid conditions for ZnBAIm. Breakthrough experiments demonstrate efficient separation of a C2H6/C2H4 (50/50, v/v) binary gas mixture under ambient conditions; more importantly, the C2H6/C2H4 separation performance is unaffected under highly humid conditions (up to 80% RH). The separation performance is attributed to combined thermodynamic (stronger dispersion interaction with C2H6 than with C2H4) and kinetic factors (diffusion), determined by density functional theory calculations and kinetic adsorption study, respectively.