Abstract

AbstractConstruction of a molecular system in which the magnetic lattice exhibits long‐range order is one of the fundamental goals in materials science. In this study, we demonstrate the artificial construction of a ferrimagnetic lattice by doping electrons into acceptor sites of a neutral donor/acceptor metal–organic framework (D/A‐MOF). This doping was achieved by the insertion of Li‐ions into the D/A‐MOF, which was used as the cathode of a Li‐ion battery cell. The neutral D/A‐MOF is a layered system composed of a carboxylate‐bridged paddlewheel‐type diruthenium(II,II) complex as the donor and a TCNQ derivative as the acceptor. The ground state of the neutral form was a magnetically disordered paramagnetic state. Upon discharge of the cell, spontaneous magnetization was induced; the transition temperature was variable. The stability of the magnetically ordered lattice depended on the equilibrium electric potential of the D/A‐MOF cathode, which reflected the electron‐filling level.

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