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Photoresponsiveness of materials is critical to their tunability and efficiency in terminal applications. Photoresponsive metal-organic polyhedra (PMOPs) feature intrinsic pores and remote controllability, but aggregation of PMOPs in solid state hampers their photoresponsiveness seriously. Herein, we report the construction of a new PMOP (Cu24(C16H12N2O4)12(C18H22O5)12, denoted as MOP-PR-LA), where long alkyl (LA) chains act as the intermolecular poles, propping against adjacent PMOP molecules to create individual microenvironment benefiting the isomerization of photoresponsive (PR) moieties. Upon ultraviolet (UV)- and visible-light irradiation, MOP-PR-LA is much easier to isomerize than the counterpart MOP-PR without LA. For propylene adsorption, MOP-PR has a low change of adsorption capacity (9.9%), while that of MOP-PR-LA reaches 58.6%. Density functional theory calculations revealed that PR in the cis state has a negative effect on adsorption, while the trans state of PR favors adsorption. This work might open an avenue for the construction of photoresponsive materials with high responsiveness and controllability.
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