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A comprehensive analysis of physical and chemical properties using the same family of spin-crossover complexes is crucial for understanding and designing structure-property relationships. However, finding an appropriate system remains challenging. Here, a series of guest-saturated states based on the 2D Hofmann-type framework [Fe(prentrz)Pd(CN)]·guest (prentrz = (1,2)-3-phenyl--(4-1,2,4-triazol-4-yl)prop-2-en-1-imine; 1·guest) is reported, exhibiting a guest-manipulated slow dynamic effect on spin equilibrium in an incomplete two-step spin-crossover (SCO) process.

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