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We report the first magnetically coupled guanidinate, α-Eu(CN3H4)2 (monoclinic, P21, a = 5.8494(3) Å, b = 14.0007(8) Å, c = 8.4887(4) Å, β = 91.075(6)°, V = 695.07(6) Å3, Z = 4). Its synthesis, polymorphism, crystal structure, and properties are complemented and supported by density-functional theory (DFT) calculations. The α-, β- and γ-polymorphs of Eu(CN3H4)2 differ in powder XRD, while the γ-phase transforms into the β-form over time. In α-Eu(CN3H4)2, Eu is octahedrally coordinated and sits in one-dimensional chains; the guanidinate anions show a hydrogen-bonding network. The different guanidinate anions are theoretically predicted to adopt syn-, anti- and all-trans-conformations. Magnetic measurements evidence ferromagnetic interactions, presumably along the Eu chains. Finally, EuC(NH)3 (isostructural to SrC(NH)3 and YbC(NH)3, hexagonal, P63/m, a = 5.1634(7) Å, c = 7.1993(9) Å, V = 166.23(4) Å3, Z = 2) is introduced as a possible ferromagnet

Synthesis, Crystal Structure, Polymorphism, and Magnetism of Eu(CN3H4)2 and First Evidence of EuC(NH)3