期刊
MOLECULES
卷 28, 期 11, 页码 -出版社
MDPI
DOI: 10.3390/molecules28114275
关键词
2,6-bis(pyrazol-3-yl)pyridine; coordination polymer; molecular design; proton-coupled electron transfer; spin crossover
Two coordination polymers were obtained through a PCET-assisted process using the hydroxy-pyrazolyl moiety of the ligand and the iron(II) ion as sources of proton and electron. Under mild conditions, the first coordination polymer of 2,6-bis(pyrazol-3-yl)pyridines was synthesized. Under harsh solvothermal conditions, a hydrogen atom transfer resulted in the transformation of hydroxyl groups, producing the third coordination polymer of 2,6-bis(pyrazol-3-yl)pyridines. This PCET-assisted approach can be used to produce coordination polymers and metal-organic frameworks with the SCO-active core N-3(L)MN3(L).
Two coordination polymers, Fe(L-3(OBF))(CH3COO)(CH3CN)(2)](n)center dot nCH(3)CN and [Fe(LO-)(2)AgNO3BF4 center dot CH3OH](n)center dot 1.75nCH(3)OH center dot nH(2)O (LO- = 3,3 '-(4-(4-cyanophenyl)pyridine-2,6-diyl)bis(1-(2,6-dichlorophenyl)-1H-pyrazol-5-olate)), were obtained via a PCET-assisted process that uses the hydroxy-pyrazolyl moiety of the ligand and the iron(II) ion as sources of proton and electron, respectively. Our attempts to produce heterometallic compounds under mild conditions of reactant diffusion resulted in the first coordination polymer of 2,6-bis(pyrazol-3-yl)pyridines to retain the core N-3(L)MN3(L). Under harsh solvothermal conditions, a hydrogen atom transfer to the tetrafluoroborate anion caused the transformation of the hydroxyl groups into OBF3 in the third coordination polymer of 2,6-bis(pyrazol-3-yl)pyridines. This PCET-assisted approach may be applicable to produce coordination polymers and metal-organic frameworks with the SCO-active core N-3(L)MN3(L) formed by pyrazolone- and other hydroxy-pyridine-based ligands.
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