Magnetic coupling between metal spins through the 7,7,8,8-tetracyanoquinodimethane (TCNQ) dianion.

A family of magnetic metal-organic frameworks, (Ph3PMe)(2)[M-2(TCNQ)(3)] {M=Fe2+, Co2+, Ni2+ and Zn2+} have been prepared and structurally characterized. The honeycomb-like "layers" consist of M-II ions doubly bridged with dinitrilomethane moieties of two 7,7,8,8-tetracyanoquinodimethane (TCNQ) dianions which are further connected through phenyl rings to form a 3D dianionic framework [M(2)TCNQ(3)](2-) with Ph3PMe+ cations filling cavities that run along the c axis. Studies of the magnetic coupling through the TCNQ dianion in these structures revealed that it can promote long-range magnetic ordering despite the long coupling pathway.