Reversible structural change of [Co2Fe2] complexes between diamagnetic hydrogen-bonded 1D chains and paramagnetic complexes within a layered structure of amphiphilic anions.

The combination of amphiphilic ions and metal complexes may enable the construction of assemblies in which the assembly structure and electronic state of the metal complexes change concertedly. In this work, an alternating layered structure of [Co2Fe2] complexes and amphiphilic anions was constructed. In the crystal structure, [Co2Fe2] complexes and water molecules formed a hydrogen-bonded supramolecular one-dimensional (1D) chain in the hydrophilic layer. A reversible structural change between the 1D chain and discrete [Co2Fe2] complexes was found to occur concertedly with an electron transfer-coupled spin transition (ETCST) of the [Co2Fe2] complex and desorption/adsorption of water molecules.