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Ancillary Ligand Effect on Single-Site Styrene Polymerization: Isospecificity of Group 4 Metal Bis(phenolate) Catalysts
2003
Styrene is polymerized isospecifically by group 4 metal complexes that contain a C2-symmetrically coordinated 1,4-dithiabutane-linked bis(phenolato) ligand activated by methylaluminoxane.
Computational Study on Cesium Azide Trapped in a Cyclopeptidic Tubular Structure
2008
The structures and the electronic properties of host-guest complexes formed by a cyclopeptidic tubular aggregate and the species CsN3, CS2(N-3)(2), and CS2N6 have been investigated by means of density functional theory. Taking advantage of the azide property to act as a bridge ligand between two or more metal cations, it may be possible to trap N-3(-) ions inside a confined space. This could be important for the preparation of polynitrogen molecules N-n. Results show that there are significant attractive interactions between the azide ion and the cavity walls, which make the ion stay inside the inner empty space of the cyclopeptidic aggregate. The confinement of the species CS2(N-3)(2) forc…
The first member of a second generation family of ligands derived from metal-ion assisted reactivity of di-2,6-(2-pyridylcarbonyl)pyridine: Synthesis…
2012
Abstract Nucleophilic attack by the carbanion −CH2COCH3 at the carbonyl carbon atoms of 2,6-di-(2-pyridylcarbonyl)pyridine, pyCOpyCOpy, in the presence of Mnn+ ions under basic conditions has yielded the cationic cluster [Mn4(OH)2(L)2(H2O)2](ClO4)4 (1), where L2− is the (py)C(CH2COCH3)(O−)(py)C(CH2COCH3)(O−)(py) dianion. The cluster cation possesses a planar {MnII2MnIII2(μ3-OH)2(μ-OR)4}4+ rhombus core, resulting from two μ3-OH− ions and two η1:η2:η1:η1:η1:η2:η1:μ3 bridging L2− groups from the in situ formed ligand. Complex 1 is antiferromagnetically coupled with an unusual S = 2 ground state resulting from spin frustration effects within the triangular Mn3 subunits of the cluster.
A 4-tert-butylcalix[4]arene tetrahydroxamate podand based on the 1-oxypiperidine-2-one (1,2-PIPO−) chelate. Self-assembly into a supramolecular ionop…
2014
An octadentate tetrahydroxamic calix[4]arene podand incorporating 1-hydroxypiperidine-2-one (1,2-PIPOH) binding units has been designed as a specific chelator for tetravalent metal cations like Zr4+ or Hf4+. This receptor, which can be considered as the first ever abiotic ligand possessing only cyclic six-membered hydroxamate groups, has been synthesized and characterized in its tetraprotonated form (1H4). Contrary to expectation, however, this new chelator did not form a 1 : 1 complex upon reaction with M(acac)4 (M = Zr and Hf; acac = acetylacetonate), but rather self-assembled into a dimeric species of 2 : 2 stoichiometry. The latter could be characterized in solution by mass spectrometry…
Postsynthetic Improvement of the Physical Properties in a Metal-Organic Framework through a Single Crystal to Single Crystal Transmetallation
2015
As ingle crystal to single crystal transmetallation process takes place in the three-dimensional (3D) metal- organic framework (MOF) of formula Mg II 2{Mg II 4(Cu II 2- (Me3mpba)2)3}·45 H2 O( 1 ;M e 3mpba 4¢ = N,N'-2,4,6-trimethyl- 1,3-phenylenebis(oxamate)). After complete replacement of the Mg II ions within the coordination network and those hosted in the channels by either Co II or Ni II ions, 1 is transmetallated to yield two novel MOFs of formulae Co2 II {Co II 4(Cu II 2(Me3- mpba)2)3}·56 H2 O( 2 )a nd Ni2 II {Ni II 4(Cu II 2(Me3mpba)2)3}· 54 H2 O( 3). This unique postsynthetic metal substitution affords materials with higher structural stability leading to enhanced gas sorption and m…
A Bis(mu-phenoxo)-Bridged Dizinc Complex with Hydrolytic Activity
2013
The dinuclear complex [Zn2(papy)2]·2CH3OH [H2papy = N- (2-hydroxybenzyl)-N-(2-picolyl)glycine] was synthesized and characterized. The crystal structure of the complex reveals that both ZnII ions are pentacoordinate with distorted pentagonal bipyramidal coordination arrangements. The phenoxyl groups of each ligand bridge the two metal atoms, whereas each carboxylate of the ligand is terminally bound to one ZnII ion. Potentiometric studies of the ZnII:H2papy system in a methanol/water mixture show the existence of a mononuclear species at lower pH; but at a pH above 5, a dimeric species starts to dominate and transforms further into a bis(μ-phenoxo) bridged dizinc complex by deprotonation of …
Electron paramagnetic resonance and magnetic circular dichroism of Gd3+ ions in oxyfluoride glass–ceramics containing CaF2 nanocrystals
2015
Abstract Magnetic resonance investigations of the Gd3 + centre structure in the oxyfluoride glass and glass–ceramics (GCs) have been carried out. The electron paramagnetic resonance (EPR) measurements showed the presence of low symmetry Gd3 + centres in the glass sample. The cubic Gd3 + centre appeared in the glass–ceramics after heat treatment of the samples at temperatures above 650 °C. The magnetic circular dichroism (MCD) measurements of both glass and glass–ceramics showed wide absorption band around 310 nm. In the GC samples MCD–EPR of the cubic Gd3 + centre has been detected.
XAFS studies of local atomic structure of niobium tellurides
1997
Abstract We present XAFS (K-edge) studies of the local atomic structure around the Nb and Te ions in niobium tellurides (NbTe 2 , Nb 3 Te 4 and NbTe 4 ) in comparison with ZrTe 2 . Using a multi-shell best-fit analysis procedure, we have reconstructed local environments of the Nb and Te ions and compared them with the existing structural models. We found that at the Nb K-edge the XAFS data of NbTe 4 are extremely sensitive to metal clustering and to the subsequent departure from the average crystallographic positions. Moreover, at the Te K-edge the XAFS data allowed us to distinguished the different type of TeTe bonds, for instance: the dimer (TeTe: 2.9 A) and the squares (TeTe: 3.3 A) i…
Computer simulations of electron paramagnetic resonance spectra of P2O5Li2WO4Li2O glasses
1992
Abstract P2O5Li2WO4Li2O glasses have been synthesized and studied over a wide range of compositions. The glasses were characterized mainly by thermodifferential analysis and electron paramagnetic resonance (EPR). The EPR spectra are characterized by the presence of two signals with very different intensities, associated with the Wv (major signal) and Mov (minor signal) paramagnetic centres. The signals have been satisfactorily reproduced by computer simulation, assuming anisotropy in the g values as well as the hyperfine parameters and linewidths. EPR parameters have been extracted and indicate metallic ions located in environments close to square pyramidal.
Electrochemical Detection of High Oxidation States of Chromium( IV and V ) in Chromium‐Doped Cassiterite and Tin‐Sphene Ceramic Pigmenting Systems
2006
Solid-state electrochemistry is applied to detect the presence of chromium centres with high oxidation states in chromium-doped cassiterite and tin-sphene ceramic pigmenting systems. Voltammetric data indicate that CrV and CrIV centres with different coordinative arrangements exist in the studied materials, and yield proton-assisted reduction processes at +0.95, +0.42 AgCl/Ag in contact with 0.50 M H2SO4. Electrochemical measurements are correlated with spectroscopic data. The CrIV and CrV metal ions display a significant light-driven electrocatalytic effect on the oxidation of 1,4-dihydrobenzoquinone and Fe(CN)64– ions that involves the formation of surface-confined adducts. (© Wiley-VCH V…