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Two metal-organic frameworks (MOFs), [Dy(BDC)(NO 3 )(DMF) 2 ]  n   ( 1 , H 2 BDC = terephthalic acid) and [Dy(BDC)(NO 3 )]  n   ( 1a ), were synthesized. The structures of MOFs  1  and  1a  are easy to be reversibly transformed into each other by the desorption or adsorption of coordination solvent molecules. Accordingly, their magnetic properties can also be changed reversibly, which realizes our goals of manipulating on/off single-molecule magnet behaviour. MOF  1  behaves as a single-molecule magnet either with or without DC field. Contrarily, no slow magnetic relaxation was observed in  1a  both under zero field and applied field.

Reversible Switching of Single-Molecule Magnetic Behaviour by Desorption/Adsorption of Solvent Ligand in a New Dy(III)-Based Metal Organic Framework