In Situ Reversible Ionic Control for Nonvolatile Magnetic Phases in a Donor/Acceptor Metal‐Organic Framework

Reversible magnetic control by electrical means, which is highly desired from the viewpoint of fundamentals and technological applications such as data storage devices, has been a challenging topic. In this study, the authors demonstrate in situ magnetic phase switching between the ferrimagnetic and paramagnetic states of an electron‐donor/‐acceptor metal‐organic framework (D/A‐MOF) using band‐filling control mediated by the Li⁺‐ion migration that accompanies redox reactions, i.e., “magneto‐ionic control”. By taking advantage of the rechargeability of lithium‐ion battery systems, in which Li⁺‐ions and electrons are simultaneously inserted into/extracted from a cathode material, the reversible control of nonvolatile magnetic phases in a D/A‐MOF has been achieved. This result demonstrates that the combination of a redox‐active MOF with porous flexibility and ion‐migration capability enables the creation of new pathways toward magneto‐electric coupling devices in the field of ionics.