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We provide a general thermodynamic framework for the understanding ofguest-induced structural transitions in hybrid organic-inorganic materials. Themethod is based on the analysis of experimental adsorption isotherms. It allowsthe determination of the free energy differences between host structuresinvolved in guest-induced transitions, especially hard to obtainexperimentally. We discuss the general case of adsorption in flexible materialsand show how a few key quantities, such as pore volumes and adsorptionaffinities, entirely determine the phenomenology of adsorption, including theoccurrence of structural transitions. On the basis of adsorptionthermodynamics, we then propose a taxonomy of guest-induced structural phasetransitions and the corresponding isotherms. In particular, we derive genericconditions for observing a double structural transition upon adsorption, oftenresulting in a two-step isotherm. Finally, we show the wide applicability andthe robustness of the model through three case studies of topical hybridorganic-inorganic frameworks: the hysteretic hydrogen adsorption inCo(1,4-benzenedipyrazolate), the guest-dependent gate-opening inCu(4,4'-bipyridine)(2,5-dihydroxybenzoate)2 and the CO2-induced "breathing" ofhybrid material MIL-53.

Thermodynamics of Guest-Induced Structural Transitions in Hybrid Organic-Inorganic Frameworks