Syntheses, Structures, and Magnetic Properties of Two DMTCNQ and DETCNQ Gadolinium Complexes

Two DMTCNQ (DMTCNQ = 2,5‐dimethyl‐7,7,8,8‐tetracyano‐ p ‐quinodimethane) and DETCNQ (DETCNQ = 2,5‐diethyl‐7,7,8,8‐tetracyano‐ p ‐quinodimethane) gadolinium complexes [Gd(DMTCNQ) 2 (CH 3 OH)(H 2 O) 6 ][DMTCNQ] · 4H 2 O ( 1 ) and [Gd(DETCNQ)(H 2 O) 7 ][2DETCNQ] ( 2 ) were synthesized by reactions of GdCl 3 · 6H 2 O with Li(DMTCNQ) or Li(DETCNQ). X‐ray diffraction analysis reveals that complexes 1 and 2 are discrete complexes. The central metal atom in 1 is coordinated by two DMTCNQ ligand radicals whereas that in 2 is coordinated by just one DETCNQ ligand radical. The adjacent molecules are connected by the intermolecular hydrogen bonds to form the two‐dimensional (2D) supramolecular layer structures, which are further packed into a three‐dimensional (3D) supramolecular architecture through the π–π interactions between ligand radicals in 1 and 2 . Magnetic investigation indicates that the antiferromagnetic interactions between spin carriers exists in 1 and 2 .