10.1021/ja066744f.s002 Konstantin I. Pokhodnya Konstantin I. Pokhodnya Michael Bonner Michael Bonner Jae-Hyuk Her Jae-Hyuk Her Peter W. Stephens Peter W. Stephens Joel S. Miller Joel S. Miller Magnetic Ordering (<i>T</i><sub>c</sub> = 90 K) Observed for Layered [Fe<sup>II</sup>(TCNE<sup>•-</sup>)(NCMe)<sub>2</sub>]<sup>+</sup>[Fe<sup>III</sup>Cl<sub>4</sub>]<sup>-</sup> (TCNE = Tetracyanoethylene) American Chemical Society 2006 TCNE FeII 90 K magnet 2006-12-13 00:00:00 Journal contribution https://acs.figshare.com/articles/journal_contribution/Magnetic_Ordering_i_T_i_sub_c_sub_90_K_Observed_for_Layered_Fe_sup_II_sup_TCNE_sup_sup_NCMe_sub_2_sub_sup_sup_Fe_sup_III_sup_Cl_sub_4_sub_sup_sup_TCNE_Tetracyanoethylene_/3041800 [Fe(TCNE)(NCMe)<sub>2</sub>][FeCl<sub>4</sub>] is isolated from the reaction of TCNE and FeCl<sub>2</sub>(NCMe)<sub>2</sub> and orders as a ferrimagnet below 90 K and is the initial member of a new class of magnets. It is the first metal−TCNE magnet with direct bonding between metal ion and [TCNE]<sup>•-</sup> whose structure has been determined, and it possesses a novel planar μ<sub>4</sub>-[TCNE]<sup>•-</sup> spin coupling unit bonded to four Fe<sup>II</sup>'s, with an axial pair of MeCNs. The [Fe<sup>III</sup>Cl<sub>4</sub>]<sup>-</sup> anion occupies sites between the [Fe<sup>II</sup>(TCNE<sup>•-</sup>)(NCMe)<sub>2</sub>]<sup>+</sup> layers. [Fe(TCNE)(NCMe)<sub>2</sub>][FeCl<sub>4</sub>] has a coercive field of 1730 Oe and a remnant magnetization of 7500 emuK/mol at 50 K.