期刊
INORGANIC CHEMISTRY
卷 55, 期 2, 页码 717-728出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.5b02159
关键词
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资金
- Platform for Drug Discovery, Informatics, and Structural Life Science from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan
- Japan Society for the Promotion of Science (JSPS) [25288038]
- PRESTO Program on Molecular Technology from the Japan Science Technology Agency (JST)
- Grants-in-Aid for Scientific Research [25288038] Funding Source: KAKEN
Solutions of 3d metal ion salts, M(NO3)(2), 4-(N-tert-butyloxylamino)pyridine (4NOpy), and dicyanamide (DCA) in CH3CN were mixed to afford single crystals of the polymeric complexes [MII(4NOpy)(x)(DCA)(y)(CH3CN)z](n) ((MI)(I) = Mn (1), Co (2), Ni (3), Cu (4a and 4b), Zn (5)). X-ray crystallography revealed that the crystal structures are a three-dimensional (3-D) network for 1, 2-D networks for 2, 3, 4a, and 5, and a 1-D chain for 4b. Crystals of 2, 3, 4a, and 5 contained CH3CN molecules as crystal solvents, which were readily desorbed in the ambient atmosphere. After desorption of the CH3CN molecules, the crystal structures of 2 and 3 were confirmed to be slightly shrunk without destruction of the crystal lattice. Crystals of 2, 3, 4a, and 5 after desorption of crystal solvents were used for investigations of the magnetic properties. Complex 1 showed antiferromagnetic interactions to form a ferrimagnetic chain and exhibited the magnetic behavior of a 2-D (or 3-D) spin-canted antiferromagnet with TN = 12 K. Complex 2 containing anisotropic CoII ions also showed the behavior of a 1-D (or 2-D) spin-canted antiferromagnet with TN = 6 K. In 3, 4a, and 4b, the aminoxyl of 4NOpy ferromagnetically interacted with the metal ion with coupling constants of J(M-NO/kB) = 45, 45, and 43 K, respectively. In 5, the magnetic couplings between the aminoxyls in 4NOpy through the diamagnetic ZnII ion were weakly antiferromagntic (J(NO-NO) = -1.2 K). DCA might be a weak antiferromagnetic connector for the metal chains.
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