Synthesis and structural and spectroscopic studies of manganese complexes of pendant-arm macrocycles based on 1,4,7-triazacyclononane: crystal structures of the manganese(II) complex [MnLH3][MnCl4] and of the mixed-valence manganese(II)-manganese(IV) hydrogen-bridged dimer [MnLH3LMn][PF6]3 (LH3 = N,N',N''-tris[(2S)-2-hydroxypropyl]-1,4,7-triazacyclononane) and of the manganese(IV) monomer [MnL'][ClO4] (L'H3 = N,N',N''-tris(2-hydroxyethyl)-1,4,7-triazacyclononane)

Belal, A.A.M.; Chaudhuri, Phalguni; Fallis, Ian A.; Farrugia, Louis J.; Hartung, Robert; Macdonald, Norman M.; Nuber, Bernhard; Peacock, Robert D.; Weiß, Johannes; Weighardt, Karl

doi:10.1021/ic00023a022

Cited by 43 publications

(22 citation statements)

References 6 publications

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“…19 although these ligands also formed octahedral co-ordination geometries in a (Mn II , Mn IV ) hydrogen-bridged dimer. 20, 21 More recently, Ward, McCleverty et al showed that the ligand tris(pyrazolylpyridyl)borate (Tp py ; Fig. 4) can be co-ordinated to tetrahedral Ag I to give trinuclear species, 22 Zn II and Mn II to give tetrameric [M 4 L 4 ] 4+ octahedral complexes 23 or with Co II to give the monomeric trigonal prismatic species, [Co(Tp py )][PF 6 ].…”

Section: Introductionmentioning

confidence: 99%

A novel bipyridine-based hexadentate tripodal framework with a strong preference for trigonal prismatic co-ordination geometries

et al. 2010

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The synthesis of the novel ligand tris(2,2¢-bipyrid-6-yl) methanol (L 1 ) is described. Co-ordination of the ligand to the first row transition metals (Mn 2+ -Zn 2+ ) as well as Cd 2+ showed that the ligand formed complexes close to trigonal prismatic in geometry in the solid state. Analysis of the geometry of the co-ordination spheres showed varying degrees of trigonal prismatic and octahedral character. For each d-electron configuration, this could be related to the relative differences in ligand field stabilisation energies for the two geometries.

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Section: Introductionmentioning

confidence: 99%

A novel bipyridine-based hexadentate tripodal framework with a strong preference for trigonal prismatic co-ordination geometries

et al. 2010

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“…The THP ligand, which contains OH ligators, is interesting because it can form complexes in which the OH can remain protonated and act as an alcohol or can deprotonate and act as an alkoxide . Mass spectrometry in the ESI‐positive mode in CH 3 OH was able to demonstrate the nuclearity of I and II .…”

Section: Resultsmentioning

confidence: 99%

“…Peacock et al . have reported that the structure of the Co(III) and Mn(III) complexes with L΄H 3 (L΄H 3 = N,N΄,N΄΄‐tris[2‐hydroxypropyl]‐l,4,7‐triazacyclononane) are very similar to the ligand of THP, which occurs as a hydrogen‐bridged dimer [Co(L΄H 3 )(L΄)Co] 3+ and [Mn(L΄H 3 )(L΄)Mn] 3+ . Under mildly basic conditions (water at pH 7 is sufficient), every second mole of ligand L΄H 3 deprotonates, and aerial oxidation produces the mixed valence dimer [M(L΄H 3 )(L΄)M] 3+ .…”

Section: Resultsmentioning

confidence: 99%

Two heptadentate Co(III) and Mn(III) complexes with partially deprotonated cyclen derivative bearing four hydroxypropyl pendants: structure, DNA binding and DNA cleavage

Yin

Wen

Geng

et al. 2012

Applied Organom Chemis

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4,7,10-tetra-(2-hydroxypropyl)-l,4,7,10-tetraazacyclododecane] using electrospray ionization mass spectrometry and X-ray photoelectron spectrometery. The characterizations confirmed that the valences of the metal ions increased from divalent to trivalent due to deprotonation of one OH group (H 4 L was in the form of H 3 L À ). Owing to the instability of Co(III) and Mn(III) in both air and in solution, they preferred to exist in divalent form. The two heptadentate complexes are extraordinary in that the chiral pendants of the complexes are different in configuration. Spectroscopic studies, viscosity measurements, thermal denaturation experiments and circular dichroism spectra demonstrated that the complexes were prone to interact with DNA by groove binding. At micromolar concentrations and under physiological conditions, the two complexes were able to oxidatively cleave the supercoiled pUC19 plasmid DNA into its nicked and linear forms. Mechanistic studies using various additives suggest the complexes had structures different from those of other inorganic complexes. These are the first reported inorganic complexes not containing planar aromatic ligands and yet binding at the major groove.

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“…Compound 2 showed electrochemical behavior consistent with previously reported mixed-valent manganese complexes (Figure 5b). [47][48][49][50] A reversible reduction is observed at -0.508 V that is attributed to the reduction process of Mn III to Mn II . Repetitive cyclic voltammetry scans confirmed the reversibility of the process ( Figure S5).…”

Section: X-ray Crystallographic Analysis Of Nanocapsules 1 Andmentioning

confidence: 99%

Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal–Organic Nanocapsules

et al. 2018

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Two structurally analogous Mn-seamed C-alkylpyrogallol[4]arene (PgC )-based metal-organic nanocapsules (MONCs) have been synthesized under similar reaction conditions and characterized by crystallographic, electrochemical, and magnetic susceptibility techniques. Both MONCs contain 24 Mn centers, but, somewhat surprisingly, marked differences in oxidation state distribution are observed upon analysis. One MONC contains exclusively Mn ions, while the other is a mixed-valence Mn/ Mn assembly. We propose that these disparate oxidation state distributions arise from slight differences in pH achieved during synthesis, a factor that may lead to many spectacular new MONCs (and associated host-guest chemistries).

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Cited by 43 publications

References 6 publications

A novel bipyridine-based hexadentate tripodal framework with a strong preference for trigonal prismatic co-ordination geometries

A novel bipyridine-based hexadentate tripodal framework with a strong preference for trigonal prismatic co-ordination geometries

Two heptadentate Co(III) and Mn(III) complexes with partially deprotonated cyclen derivative bearing four hydroxypropyl pendants: structure, DNA binding and DNA cleavage

Oxidation State Distributions Provide Insight into Parameters Directing the Assembly of Metal–Organic Nanocapsules

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