期刊
CRYSTAL GROWTH & DESIGN
卷 14, 期 2, 页码 477-490出版社
AMER CHEMICAL SOC
DOI: 10.1021/cg401141a
关键词
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资金
- Young Scientist Fund [21301128, 21001080]
- Natural Science Foundation of Tianjin [11JCYBJC03600]
- Tianjin Normal University [5RL090]
Based on the 4-substituted 1,2,4-triazole derivate ligand 4-benzene-1,2,4-triazole (L), a series of crystalline coordination complexes varying from mononuclear to trinuclear species, namely, [Zn(L)(2)Br-2] (I), [Zn(L)(2)Br-2] (2), [Fe(L)(4)(NCS)(2)](2) (3), [Fe-2(mu(2)-L)(3)(L)(2)(NCS)(4)]center dot CH3OH center dot CH3CH2OH (4), [Fe-2(mu(2)-L)(3)(L)(2)(NCS)(4)]center dot 2CH(3)CH(2)OH (5), [Fe-2(mu(2)-L)(3)(L)(2)(NCS)(4)]center dot 2CH(3)CH(2)OH center dot 1.5H(2)O (6), and [Ni-3(mu(2)-L)(6)(L)(4)(H2O)(2)](NO3)(6)center dot 15.5H(2)O (7), have been isolated. 1 and 2 present a temperature-induced polymorphic phenomenon of two zinc(II) coordination complexes with L. The solvent effect plays the key role for the self-assembly of these Fe(II) complexes 3-6: 3 contains mononuclear Fe(L)(4)(NCS)(2) units without spin-transition behavior, whereas both 4 and 5 present binuclear Fe(II) complexes with three N-1,N-2-1,2,4-triazole bridges exhibiting incomplete spin-transition behavior. The low-temperature X-ray structural analysis (100 K) of 4 also confirms that one of the Fe(II) centers is located at the low-spin (LS) state and the other Fe(II) center is located at the high-spin (HS) state. Interestingly, when the binuclear Fe(II) complex 5 was exposed in the water atmosphere, solvent-induced single crystal-to-single crystal transformation can be observed, and the binuclear Fe(II) complex 6 exhibiting antiferromagnetic interactions can be isolated. Further, a trinuclear crystalline compound is isolated when Ni(II) salts were used to react with L. Variable-temperature magnetic susceptibility measurement (2-300 K) reveals antiferromagnetic interactions in 7. The polymorphic phenomenon (1 and 2), incomplete spin-transition phenomenon (4 and 5), and single crystal-to-single crystal transformation (from 5 to 6) also reveal great potential in the construction of these novel functional materials with L.
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