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A series of 3d metal complexes prepared by in situ reactions of a flexible diacylhydrazine ligand: synthesis, structures and magnetic properties

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Abstract

The coordination reactions of 3d metal salts with malonic acid N,N′-bis(salicyloyl) bishydrazide (H6mbshz) afforded three complexes, namely [Cu2(H2bshz)(Py)4Cl2]·Py (1) (Py = pyridine), [Fe2(bshz)(Py)2] (2) and the known complex [Ni4(aehba)2(DMF)2(H2O)2]·2DMF (3), where bshz = N,N′-bis(salicyloyl)hydrazine anion and aehba4− = azo-enolic-2-hydroxybenzamide anion. The X-ray crystal structures of all three complexes have been obtained. Complexes 1 and 2 are composed of N–N-bridged binuclear units, while complex 3 displays a planar tetranuclear structure in which four Ni(II) centers are linked together by N–N and N=N bonds. The bshz anions in 1 and 2 and aehba4− anions in 3 were all generated in situ from H6mbshz. A mechanism for these reactions is proposed, involving tandem C–N cleavage and C–N/N–N coupling processes via free radical intermediates. Magnetic investigations revealed dominant antiferromagnetic interactions between the metallic centers of each complex.

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Acknowledgments

This work was supported by the National Natural Science Foundation of China (Nos. 51572050, 21271050 and 21261004) and the Guangxi Natural Science Foundation (Nos. 2015GXNSFDA 139007, 2014GXNSFBA118055 and 2013GXNSFGA019008).

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Authors and Affiliations

  1. Guangxi Key Laboratory of Electrochemical and Magnetochemical Functional Materials, College of Chemistry and Bioengineering, Guilin University of Technology, Guilin, 541004, China

    Kai Wang, Yan Li & Fu-Pei Liang

  2. State Key Laboratory for the Chemistry and Molecular Engineering of Medicinal Resources, School of Chemistry and Pharmacy, Guangxi Normal University, Guilin, 541004, China

    Zi-Lu Chen, Hua-Hong Zou & Fu-Pei Liang

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  1. Kai Wang
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  2. Zi-Lu Chen
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  3. Hua-Hong Zou
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  4. Yan Li
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Correspondence to Fu-Pei Liang.

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Wang, K., Chen, ZL., Zou, HH. et al. A series of 3d metal complexes prepared by in situ reactions of a flexible diacylhydrazine ligand: synthesis, structures and magnetic properties. Transit Met Chem 42, 17–23 (2017). https://doi.org/10.1007/s11243-016-0101-0

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  • DOI: https://doi.org/10.1007/s11243-016-0101-0

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