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  • 1
    Electronic Resource
    Electronic Resource
    Weinheim : Wiley-Blackwell
    Chemistry - A European Journal 1 (1995), S. 3-3 
    ISSN: 0947-6539
    Keywords: Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
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  • 2
    ISSN: 0947-6539
    Keywords: chlorine complexes ; ethene complexes ; intermediates ; rotational spectroscopy ; Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: A complex of ethene and Cl2 has been characterised in the gas phase. Rotational spectra of the isotopomers C2H4…35Cl2, C2H4…35Cl37Cl and C2H4…37Cl35Cl were recorded by using a fast-mixing nozzle in an FT microwave spectrometer. Rotational constants, centrifugal distortion constants and Cl nuclear quadrupole coupling constants. χgg (Cl) are reported in each case. The complex is of the π-donor-acceptor type and has a C2v geometry in which Cl2 lies along the C2 axis perpendicular to the plane of the C2H4 nuclei. The binding is weak, and only small changes in the χgg (Cl) attend complex formation. A simple model attributes these changes to a transfer of around 0.02e from the inner to the outer Cl nucleus, thus confirming that the complex is of the Mulliken outer type. Similarities in the properties of C2H4… Cl2 and C2H4… HCl indicate that the angular geometry is in both cases determined mainly by the electrostatic part of the interaction. The distance from the π-bond midpoint to Cl decreases from C2H4… HCl to C2H4… Cl2; this suggests that Cl2 is “snub-nosed”.
    Additional Material: 5 Ill.
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  • 3
    Electronic Resource
    Electronic Resource
    Weinheim : Wiley-Blackwell
    Chemistry - A European Journal 1 (1995), S. 7-11 
    ISSN: 0947-6539
    Keywords: density-functional calculations ; ion-molecule reactions ; relativistic effects ; thermochemistry ; uranium compounds ; Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The nitridooxouranium cation NUO+ has been prepared as a new isoelectronic homologue to the uranyl dication UO22+ by a sequence of ionmolecule reactions starting from the atomic uranium cation U+. Collision-induced dissociation experiments and ligand-exchange reactions serve to unambiguously identify the ion as a species in which the uranium cation is formally inserted in the NO molecule. New thermochemical data for NUO+ and UN+ are given, and the stability of NUO+ with respect to UO22+ is investigated by means of quasi-relativistic density-functional calculations.
    Additional Material: 3 Ill.
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  • 4
    ISSN: 0947-6539
    Keywords: amethyrin ; orangarin ; porphyrinoids ; terpyrroles ; Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: A new, general synthesis of the first β-substituted tetra- and hexaalkyl terpyrroles is described. Also described are two new classes of expanded porphyrins derived from the hexaalkyl terpyrrole. The key step in the terpyrrole formation is the copper(II)-mediated oxidative coupling of the LDA-derived enolates of α-keto pyrroles. The first new expanded porphyrin reported here, the so-called “orangarin”, contains five pyrrolic subunits and two bridging carbon atoms, and is formally a 20π-electron nonaromatic macrocycle. The second new class of expanded porphyrins, the “amethyrins”, are 24π-electron nonaromatic macrocycles containing six pyrrole units. Both of these new macrocycles, as well as one of the new terpyrrolic precursors have been structurally characterized by single crystal X-ray diffraction analysis.
    Additional Material: 12 Ill.
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  • 5
    ISSN: 0947-6539
    Keywords: porphyrinoids ; Rothemund synthesis ; sapphyrin ; Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: The Rothemund-type condensation of pyrrole and benzaldehyde yields, apart from 5,10,15,20-tetraphenylporphyrin (TPPH2) and inverted tetraphenylporphyrin 2-aza-21-carba-5,10,15,20-tetraphenylporphyrin (CTPPH2), a unique pentapyrrolic macrocyclic molecule with the aromatic nucleus of sapphyrin, namely, 5,10,15,20-tetraphenylsapphyrin (TPSH3). Its unorthodox structural skeleton with an inverted pyrrole ring lying opposite to the bipyrrole unit accounts for the spectroscopic properties of the novel sapphyrin. The diprotonation of TPSH3 acts as a trigger for a structural transformation involving a flip of the pyrrole units, which relocates the 27-NH pyrrolic nitrogen from the periphery into the center of the macrocycle. The formation of 5,10,15,20-tetraphenylsapphyrin proves that the pentapyrrolic product is accessible by the mechanism of the Rothemund synthesis.
    Additional Material: 5 Ill.
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  • 6
    ISSN: 0947-6539
    Keywords: catenanes ; cyclodextrins ; macrocycles ; orientational isomerism ; Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: A novel synthetic approach is described for the construction of catenanes in aqueous solution from a partially methylated cyclodextrin (CD)-namely, heptakis(2,6-di-O-methyl-β-cyclodextrin) (DM-β-CD)-and a range of substrate molecules that contain a hydrophobic central core in the form of a 4,4′-disubstituted biphenyl unit (usually bitolyl) carrying two hydrophilic polyether side chains terminated by primary amine functions. In water, the amphiphilic catenane precursors form 1:1 complexes with β-CD and DM-β-CD and 2:1 (guest: host) complexes with the larger γ-CD. Macrocyclizations of the biphenyl-containing substrates with aromatic diacid chlorides in aqueous solution and in the presence of DM-β-CD under Schotten-Baumann conditions afforded-in low yields-a range of [2]- and [3]catenanes. When a consitutionally asymmetrical diamine was employed as the substrate, orientational isomers of a [2]catenane were obtained. A [3]catenene incorporating a macrocyclic tetralactam was found to exist as a mixture of head-to-head and head-to-tail isomers, which could be separated by high pressure liquid chromatography and identified unambiguously by nuclear magnetic resonance spectroscopy. One of the [2]catenanes afforded good single crystals from which the solid state structure was determined by X-ray crystallography. Other techniques which aided the characterization of these novel compounds included ultraviolet/visible and luminescence spectroscopy, dynamic nuclear magnetic resonance spectroscopy and fast atom bombardment mass spectrometry. Generally speaking, the catenated cyclodextrins are soluble in halogenated and aromatic hydrocarbons as well as in hydroxylic solvents. The existence of these new compounds gives us a unique insight into the nature of the noncovalent bonding interactions that cyclodextrins employ in binding substrate molecules.
    Additional Material: 29 Ill.
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  • 7
    ISSN: 0947-6539
    Keywords: chelate ligands ; hydrogen bonds ; ligand design ; mass spectrometry ; stability constants ; Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: A series of compounds containing the mononuclear complexes [M(tdci)2]3+ (tdci = 1,3,5-trideoxy-1,3,5-tris(dimethylamino)-cis-inositol, M = Al, Fe, Ga, In) and [M(tdci)2]4+ (M = Ti, Ge, Sn) was prepared and characterized by elemental analysis, NMR spectroscopy, and FAB mass spectrometry. Characteristic fragmentation reactions in the mass spectra were elucidated. X-ray analysis of the AlIII, FeIII, GaIII, and InIII complexes revealed that two neutral, zwitterionic tdci ligands coordinate to the metal cation exclusively through deprotonated alkoxo groups. The six coordinated oxygen donors and the six N—H protons form a hydrophilic pocket, whereas the two cyclohexane rings and the twelve methyl groups form two hydrophobic shells. The hydrophilic pocket is filled with twelve water molecules, which are arranged as a second and a third coordination sphere around the metal cation. The reactivity in aqueous solution was investigated by potentiometric measurements. The bis complexes proved to be stable at pH 7. The evaluated formation constants show an increase of stability in the order AlIII〈InIII〈GaIII〈FeIII. The measurements established that tdci is one of the most effective tridentate ligands for small (r ≤ 0.8Å) and highly charged cations. The different chelating properties of tdci and of the unmethylated 1,3,5-triamino- 1,3,5-trideoxy-cis-inositol are discussed in terms of different steric requirements and different types of solvation of the corresponding complexes in aqueous solution.
    Additional Material: 10 Ill.
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  • 8
    Electronic Resource
    Electronic Resource
    Weinheim : Wiley-Blackwell
    Chemistry - A European Journal 1 (1995), S. cpi 
    ISSN: 0947-6539
    Keywords: Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
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  • 9
    ISSN: 0947-6539
    Keywords: charge transfer ; EPR spectroscopy ; organometallic compounds ; platinum compounds ; spectroelectrochemistry ; Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Notes: In spite of their very similar cyclic voltammograms, absorption spectra, and solvatochromic behavior, the two 1,4-diazabutadiene title complexes exhibit markedly different photoreactivities and underlying electronic structures, as evident from absorption and EPR spectra of the persistent anion radical forms. The lowest excited state of the nonphotoreactive PtII system [(CyN=CH—CH=NCy)-PtMe2] has MLCT (metal-to-ligand charge-transfer, 5d → π*) character, and the EPR spectrum of the corresponding anion radical at 〈g〉 = 2.016 exhibits sizable metal/ligand orbital mixing. On the other hand, the structurally characterized PtIV complex [(CyN=CH—CH=NCy)-PtMe4] (C2/c; a = 2021.6(2), b = 805.3(1), c = 1254.2(1) pm; β = 111.05(1)°; V = 1905.7(4) × 106 pm3; Z = 4) has a lowlying photoreactive LLCT (ligand-to-ligand charge-transfer, σPt—C → π*) excited state in which the axial Pt—C bonds are activated, as already suggested by the longer Pt—C(ax) bonds (214.0(8) pm) relative to Pt—C(eq) in the ground state (204.5(5) pm). The anion radical of the PtIV complex has lost the long-wavelength absorption band in the visible; it shows a well-resolved EPR spectrum at 〈g〉 = 1.9945 with π-ligand and 195Pt hyperfine structure and a small g anisotropy. A qualitative MO scheme is presented to account for the similar frontier-orbital energy differences despite dissimilar underlying electronic structures.
    Additional Material: 7 Ill.
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  • 10
    Electronic Resource
    Electronic Resource
    Weinheim : Wiley-Blackwell
    ISSN: 0947-6539
    Keywords: Chemistry ; General Chemistry
    Source: Wiley InterScience Backfile Collection 1832-2000
    Topics: Chemistry and Pharmacology
    Type of Medium: Electronic Resource
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