Synthesis, X-ray crystal structures, magnetism, and phosphate ester cleavage properties of copper(II) complexes of N-substituted derivatives of 1,4,7-triazacyclononane

Inorganic Chemistry
Matthew J BelousoffLeone Spiccia

Abstract

Two new N-substituted derivatives of the 1,4,7-triazacyclononane (tacn) macrocycle, 1-benzyl-4,7-dimethyl-1,4,7-triazacyclononane (L2) and 1,4,7-tris(3-cyanobenzyl)-1,4,7-triazacyclononane (L3), have been prepared and, together with 1,4-dimethyl-1,4,7-triazacyclononane (L1), have been used to synthesize the corresponding hydroxo-bridged binuclear copper (II) complexes, [Cu2(mu-OH)2L2](ClO4)2.xH2O (1 L = L1, x = 0; 2 L = L2, x = 1; 3 L = L3, x = 2). The X-ray crystal structures of all three complexes reveal the presence of [Cu2(mu-OH)2]2+ cores capped by pairs of facially coordinating tacn ligands so that the Cu(II) centers reside in distorted square pyramidal coordination environments. Variable-temperature magnetic susceptibility measurements indicate weak antiferromagnetic coupling (J = -36.4 cm(-1)) between the Cu(II) centers in 1, while the centers in 2 and 3 have been shown to interact ferromagnetically (J = 11.2 and 49.3 cm(-1), respectively). The variation in the strength and sign of these interactions has been rationalized in terms of the differing geometries of the [Cu2(mu-OH)2]2+ cores. The ability of the Cu(II) complexes to cleave phosphate ester bonds has been probed using the model phosphate ester bis(4-nitrophenyl)...Continue Reading

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Citations

Jan 6, 2009·Journal of the American Chemical Society·Matthew J BelousoffBim Graham
Aug 6, 2015·Accounts of Chemical Research·Tanmaya JoshiLeone Spiccia
Apr 18, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Emily CurnockR Nathan Williams
Aug 10, 2006·Dalton Transactions : an International Journal of Inorganic Chemistry·Alexander SchillerKay Severin
Aug 9, 2008·Dalton Transactions : an International Journal of Inorganic Chemistry·Juan HeLiang-Nian Ji
Jan 1, 2009·Acta Crystallographica. Section E, Structure Reports Online·Adailton J BortoluzziVitor C Weiss
Apr 22, 2021·Dalton Transactions : an International Journal of Inorganic Chemistry·Muhammad Usman AnwarJeremy M Rawson
Nov 6, 2013·Inorganic Chemistry·Arumugam ThangavelChristopher C Scarborough

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