Development of porous magnets with electron donor/acceptor metal–organic frameworks

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Nowadays, the control of spontaneous magnetization in the molecular magnets has been mainly actualized by photo-irradiation, solvent accommodation, or electrochemical approach. Here, we demonstrate for the first time CO2 can be adsorbed to generate the long-range magnetic order in an electronic-state-flexible layered compound, [{Ru2(2,4-F2PhCO2)4}2TCNQ(OEt)2] (1). The adsorption of CO2 into compound 1 is accompanied by a structural transformation with the bending deflection of TCNQ(OEt)2, which plays an extremely important role in controlling the electronic states. Owing to the reversible change of electronic states by the CO2 adsorption/desorption processes, magnetic phase is switched between antiferromagnetic phase (CO2-adsorbed phase) and paramagnetic phase (CO2-free phase).