Dynamic structural transformations, based on flexible porous frameworks are a major challenge in material sciences, both from a fundamental and a practical point of view. We have constructed a number of metal-organic chains, networks and frameworks based on metallocyanides. Some of these metal-organic cyano-bridged compounds (MOCB’s) show structural transformations on dehydration/rehydration. The “sponge-like” behaviour of the molecular transformations is accompanied by a colour change and it has been shown by in-situ powder X-ray diffraction and immersion calorimetry to be completely reversible. By a combination of the DSC, powder XRD and immersion calorimetry it was also possible to find the net heat of the transformation. For one such system the structural transformation, driven by solvent molecules, lead to the formation of two types of networks that show different behaviour upon drying, falling within the category of “recoverable collapsing” and “guest-induced reformation” frameworks. We will show that the synthetic strategy based on cyanide-bridged bimetallic assemblies is advantageous for the formation of flexible nanoporous materials.

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