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Reaction of 2,2'-bipyridine (2,2'-bipy) or 1,10-phenantroline (phen) with [Mn(Piv) 2 (EtOH)]  n  led to the formation of binuclear complexes [Mn 2 (Piv) 4 L 2 ] (L = 2,2'-bipy ( 1 ), phen ( 2 ); Piv - is the anion of pivalic acid). Oxidation of 1 or 2 by air oxygen resulted in the formation of tetranuclear Mn II/III complexes [Mn 4 O 2 (Piv) 6 L 2 ] (L = 2,2'-bipy ( 3 ), phen ( 4 )). The hexanuclear complex [Mn 6 (OH) 2 (Piv) 10 (pym) 4 ] ( 5 ) was formed in the reaction of [Mn(Piv) 2 (EtOH)]  n  with pyrimidine (pym), while oxidation of 5 produced the coordination polymer [Mn 6 O 2 (Piv) 10 (pym) 2 ]  n  ( 6 ). Use of pyrazine (pz) instead of pyrimidine led to the 2D-coordination polymer [Mn 4 (OH)(Piv) 7 (µ 2 -pz) 2 ]  n  ( 7 ). Interaction of [Mn(Piv) 2 (EtOH)]  n  with FeCl 3 resulted in the formation of the hexanuclear complex [Mn II  4 Fe III  2 O 2 (Piv) 10 (MeCN) 2 (HPiv) 2 ] ( 8 ). The reactions of [MnFe 2 O(OAc) 6 (H 2 O) 3 ] with 4,4'-bipyridine (4,4'-bipy) or trans -1,2-(4-pyridyl)ethylene (bpe) led to the formation of 1D-polymers [MnFe 2 O(OAc) 6 L 2 ]  n  ·2 n DMF, where L = 4,4'-bipy ( 9 ·2DMF), bpe ( 10 ·2DMF) and [MnFe 2 O(OAc) 6 (bpe)(DMF)]  n  ·3.5 n DMF ( 11 ·3.5DMF). All complexes were characterized by single-crystal X-ray diffraction. Desolvation of 11 ·3.5DMF led to a collapse of the porous crystal lattice that was confirmed by PXRD and N 2 sorption measurements, while alcohol adsorption led to porous structure restoration. Weak antiferromagnetic exchange was found in the case of binuclear Mn II complexes ( J Mn-Mn  = -1.03 cm -1 for 1 and 2 ). According to magnetic data analysis ( J Mn-Mn  = -(2.69 ÷ 0.42) cm -1 ) and DFT calculations ( J Mn-Mn  = -(6.9 ÷ 0.9) cm -1 ) weak antiferromagnetic coupling between Mn II ions also occurred in the tetranuclear {Mn 4 (OH)(Piv) 7 } unit of the 2D polymer 7 . In contrast, strong antiferromagnetic coupling was found in oxo-bridged trinuclear fragment {MnFe 2 O(OAc) 6 } in 11 ·3.5DMF ( J Fe-Fe  = -57.8 cm -1 , J Fe-Mn  = -20.12 cm -1 ).

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Versatile Reactivity of MnII Complexes in Reactions with N-Donor Heterocycles: Metamorphosis of Labile Homometallic Pivalates vs. Assembling of Endurable Heterometallic Acetates