In this paper, we report a two-dimensional (2D) Hofmann-type spin-crossover coordination polymer [Fe(-NTrz)Pt(CN)]·HO (-NTrz = 4-(-nitrobenzyl)imino-1,2,4-triazole). Due to the remarkable configurational flexibility of triazole-based ligand, the porous structure of this compound can be reversibly regulated by the loss of guest water molecules as a consequence of rotation of -NTrz. The 180° reorientation of the -nitrobenzyl moiety not only induces a response of gate-closing/opening of the porous framework but also significantly modulates the spin transition temperature. The present investigation highlights the potential of Hofmann-type SCO compounds with flexible ligands in exploring unusual physical and chemical phenomena.
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