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Issue 27, 2015
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Synthesis, structural studies, kinetic stability, and oxidation catalysis of the late first row transition metal complexes of 4,10-dimethyl-1,4,7,10-tetraazabicyclo[6.5.2]pentadecane

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Abstract

Synthetic details for 4,11-dimethyl-1,4,8,11-tetraazabicyclo[6.5.2]pentadecane, the dimethyl ethylene cross-bridged homocyclen ligand are presented for the first time. Its novel Mn2+, Fe2+, Mn3+, and Fe3+ complexes have been synthesized and characterized. X-ray crystal structures were obtained for both manganese complexes, along with five additional Co3+, Cu2+, and Zn2+ structures, the first structural characterization of complexes of this ligand. Each complex has the cis-V configuration of the cross-bridged macrocycle ring, leaving cis labile binding sites for interaction of the complex with oxidants and/or substrates. The copper(II) complex kinetic stability in 5 M HCl and at elevated temperatures was determined and compared to related complexes in the literature. The electronic properties of the manganese and iron complexes were evaluated using solid state magnetic moment determination and acetonitrile solution electronic spectroscopy, revealing high spin metal complexes in all cases. Cyclic voltammetry in acetonitrile of the divalent iron and manganese complexes revealed reversible redox processes, suggesting catalytic reactivity involving electron transfer processes are possible for both complexes. Screening of the Mn2+ and Fe2+ complexes for oxidation catalysis using hydrogen peroxide as the terminal oxidant showed both complexes are worthy of continued development.

Graphical abstract: Synthesis, structural studies, kinetic stability, and oxidation catalysis of the late first row transition metal complexes of 4,10-dimethyl-1,4,7,10-tetraazabicyclo[6.5.2]pentadecane

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Supplementary files

Article information


Submitted
19 Feb 2015
Accepted
01 Apr 2015
First published
15 Apr 2015

Dalton Trans., 2015,44, 12210-12224
Article type
Paper

Synthesis, structural studies, kinetic stability, and oxidation catalysis of the late first row transition metal complexes of 4,10-dimethyl-1,4,7,10-tetraazabicyclo[6.5.2]pentadecane

D. L. Matz, D. G. Jones, K. D. Roewe, M. Gorbet, Z. Zhang, Z. Chen, T. J. Prior, S. J. Archibald, G. Yin and T. J. Hubin, Dalton Trans., 2015, 44, 12210
DOI: 10.1039/C5DT00742A

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