A series of six cyanide-bridged heterobimetallic complexes including {[M(L)2]2[Mn(TPP)]}[Mn(TPP)(MeOH)2]·xH2O·yMeOH {L = 1,2-bis(pyridine-2-carboxamido)-4-methylbenzenate (bpb2−), M = Cr (1), Co (2); L = 1,2-bis(pyridine-2-carboxamido)benzenate (bpmb2−), M = Cr (3), Co (4); TPP = meso-tetra(phenyl)porphyrin} and {[M(bpb)(CN)2][Mn(TClPP)(MeOH)]}·xH2O·yMeOH {M = Cr (5), Co (6), TClPP = meso-tetra(4-chlorophenyl)porphyrin} were designed and synthesized with two manganese(III)–porphyrin compounds and four pyridinecarboxamide dicyanidemetalates as building blocks. X-ray diffraction analysis reveals that compounds 1–4 containing the [Mn(TPP)]+ ion connect two dicyanide-containing [M(L)(CN)2]− anions to form the anionic trinuclear sandwich-like MIII–MnIII–MIII molecular moiety with the one [Mn(TPP)(CH3OH)2]+ segment as a balance cation. The MIII–MnIII complexes 5 and 6 show a dinuclear molecular conformation comprised of [M(bpb)(CN)2]− and [Mn(TClPP)(MeOH)]+ ions bridged by one cyanide group linking the MnIII ion. Investigation of magnetic properties of the cyanide-bridged Cr–Mn complexes reveals the weak antiferromagnetic interaction between MnIII and CrIII magnetic centers with JMnCr = −0.116(2), −0.092(2) and −0.86(2) cm−1 for 1, 3, and 5, respectively.
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