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The guest-dependent flexibility of the pillared-layered metal–organic framework (MOF), Zn 2 bdc 2 dabco· X (guest), where guest = EtOH, DMF or benzene, has been examined by high-pressure single crystal X-ray diffraction. A pressure-induced structural phase transition is found for the EtOH- and DMF-included frameworks during compression in a hydrostatic medium of the guest species, which is dependent upon the nature and quantity of the guest in the channels. The EtOH-included material undergoes a phase transition from  P 4/ mmm  to  C 2/ m  at 0.69 GPa, which is accompanied by a change in the pore shape from square to rhombus  via  super-filling of the pores. The DMF-included material undergoes a guest-mediated phase transition from  I 4/ mcm  to  P 4/ mmm  at 0.33 GPa  via  disordering of the DMF guest. In contrast, the benzene-included framework features a structure with rhombus-shaped channels at ambient pressure and shows direct compression under hydrostatic pressure. These results demonstrate the large influence of guest molecules on the high-pressure phase behavior of flexible MOFs. Guest-mediated framework flexibility is useful for engineering MOFs with bespoke pore shapes and compressibility.

Guest-mediated phase transitions in a flexible pillared-layered metal–organic framework under high-pressure