Magnetic Properties of Mixed Ligand Ni II 2 and Ni II 4 Complexes Composed of Macrocyclic Hexaamine‐Dithiophenolato and Bridging Tetrazolato Ligands

The magnetic properties of the dinuclear and tetranuclear nickel(II) tetrazolato complexes [Ni 2 L( R CN 4 )][BPh 4 ] ( R = H ( 4 ), Me ( 5 ), Ph ( 6 )) and [(Ni 2 L) 2 (1,4‐(CN 4 ) 2 ‐C 6 H 4 )][BPh 4 ] 2 ( 7 ), where (L) 2– represents a 24‐membered macrocyclic N 6 S 2 supporting ligand, are reported. Analysis of temperature‐dependent magnetic susceptibility measurements over the temperature range from 2 to 300 K revealed the presence of weak ferromagnetic exchange interactions between the Ni II ions in the binuclear [Ni 2 L(μ‐L′)] + subunits with magnetic exchange coupling constant values of J 1 = 13.5 cm –1 for 4 , J 1 = 20.0 cm –1 for 5 , J 1 = 19.2 cm –1 for 6 , and J 1 = 15.2 cm –1 for 7 ( H = –2 J S 1 S 2 ). The exchange coupling J 2 across the bistetrazolato bridge in 7 is less than 0.1 cm –1 , which suggests that no significant interdimer coupling occurs in this compound. The synthesis and crystal structure of the new complex 7 ·2MeCN is also reported.