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Berlin Brandenburg

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  • 1
    Language: English
    In: Journal of the American Chemical Society, 05 February 2014, Vol.136(5), pp.2094-100
    Description: We report on the design, synthesis, and operation of a bimetallic molecular biped on a three-foothold track. The "walker" features a palladium(II) complex "foot" that can be selectively stepped between 4-dimethylaminopyridine and pyridine ligand sites on the track via reversible protonation while the walker remains attached to the track throughout by means of a kinetically inert platinum(II) complex foot. The substitution pattern of the three ligand binding sites, together with the kinetic stability of the metal-ligand coordination bonds, affords the two positional isomers a high degree of metastability, meaning that altering the chemical state of the track does not automatically instigate stepping in the absence of an additional stimulus (heat in the presence of a coordinating solvent). The use of metastable metal complexes for foot-track interactions offers a promising alternative to dynamic covalent chemistry for the design of small-molecule synthetic molecular walkers.
    Keywords: Coordination Complexes -- Chemical Synthesis ; Palladium -- Chemistry ; Platinum -- Chemistry ; Pyridines -- Chemistry
    ISSN: 00027863
    E-ISSN: 1520-5126
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  • 2
    In: Chemical Communications, 2012, Vol.48(99), pp.12059-12061
    Description: Two triarylboron-functionalized carboxylate ligands have been found to be highly effective in selective activation of Tb( iii ) and Eu( iii ) emission and enable the use of the Tb( iii ) and Eu( iii ) complexes as highly effective luminescent indicators for F and CN in solution and on a solid substrate.
    Keywords: Activation ; Emission ; Fluorides ; Indicators ; Lanthanides ; Ligands ; Luminescence ; Visual ; Miscellaneous Sciences (So) ; Components and Materials (General) (Ea);
    ISSN: 1359-7345
    E-ISSN: 1364-548X
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  • 3
    Language: English
    In: Journal of the American Chemical Society, 03 May 2017, Vol.139(17), pp.6253-6260
    Description: Many of the desirable properties of metal-organic frameworks (MOFs) can be tuned by chemical functionalization of the organic ligands that connect their metal clusters into multidimensional network solids. When these linker molecules are intrinsically fluorescent, they can pass on this property to the resultant MOF, potentially generating solid-state sensors, as analytes can be bound within their porous interiors. Herein, we report the synthesis of a series of 14 interpenetrated Zr and Hf MOFs linked by functionalized 4,4'-[1,4-phenylene-bis(ethyne-2,1-diyl)]-dibenzoate (peb) ligands, and we analyze the effect of functional group incorporation on their structures and properties. Addition of methyl, fluoro, naphthyl, and benzothiadiazolyl units does not affect the underlying topology, but induces subtle structural changes, such as ligand rotation, and mediates host-guest interactions. Further, we demonstrate that solid-state photoluminescence spectroscopy can be used to probe these effects. For instance, introduction of naphthyl and benzothiadiazolyl units yields MOFs that can act as stable fluorescent water sensors, a dimethyl modified MOF exhibits a temperature dependent phase change controlled by steric clashes between interpenetrated nets, and a tetrafluorinated analogue is found to be superhydrophobic despite only partial fluorination of its organic backbone. These subtle changes in ligand structure coupled with the consistent framework topology give rise to a series of MOFs with a remarkable range of physical properties that are not observed with the ligands alone.
    Keywords: Chemistry;
    ISSN: 00027863
    E-ISSN: 1520-5126
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  • 4
    In: Marshall, Ross J. and Kalinovskyy, Yaroslav and Griffin, Sarah L. and Wilson, Claire and Blight, Barry A. and Forgan, Ross S. (2017) Functional Versatility of a Series of Zr MOFs Probed by Solid-State Photoluminescence Spectroscopy. Journal of the American Chemical Society, 139 (17). pp. 6253-6260.
    Description: Many of the desirable properties of metal-organic frameworks (MOFs) can be tuned by chemical functionalization of the organic ligands that connect their metal clusters into multidimensional network solids. When these linker molecules are intrinsically fluorescent, they can pass on this property to the resultant MOF, potentially generating solid-state sensors, as analytes can be bound within their porous interiors. Herein, we report the synthesis of a series of 14 interpenetrated Zr and Hf MOFs linked by functionalized 4,4ʹ-[1,4-phenylene-bis(ethyne-2,1-diyl)]-dibenzoate (peb2-) ligands, and analyse the effect of functional group incorporation on their structures and properties. Addition of methyl, fluoro, naphthyl and benzothiadiazolyl units does not affect the underlying topology, but induces subtle structural changes, such as ligand rotation, and mediates host-guest interactions. Further, we demonstrate that solid-state photoluminescence spectroscopy can be used to probe these effects. For instance, introduction of naphthyl and benzothiadiazolyl units yields MOFs that can act as stable fluorescent water sensors, a dimethyl modified MOF exhibits a temperature dependent phase change controlled by steric clashes between interpenetrated nets, and a tetrafluorinated analogue is found to be superhydrophobic despite only partial fluorination of its organic backbone. These subtle changes in ligand structure coupled with the consistent framework topology give rise to a series of MOFs with a remarkable range of physical properties that are not observed with the ligands alone.
    Keywords: Q Science ; QD Chemistry
    ISSN: 0002-7863
    Source: University of Kent
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  • 5
    Language: English
    In: Organic letters, 06 April 2012, Vol.14(7), pp.1700-3
    Description: Cyclometalated Pt(II) β-diketonates are widely used as efficient luminescent materials but are typically prepared at high temperatures in low yields using excess reagents. A one-pot synthesis of these complexes is described employing stoichiometric reagents and short reaction times at ambient temperature, giving yields of up to 94%. The method is applicable to a broad range of substrates including N^C, P^C, and C^C chelate Pt(II) complexes and different β-diketonate ligands.
    ISSN: 15237060
    E-ISSN: 1523-7052
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  • 6
    Language: English
    In: Inorganic chemistry, 16 January 2012, Vol.51(2), pp.778-80
    Description: The assembly of two copper(II)-carboxylate dimer complexes appended with four peripheral triarylborane functionalities has been achieved. Complex stabilities in the presence of fluoride are examined.
    Keywords: Borane -- Chemical Properties ; Carboxyl Compounds -- Chemical Properties ; Chemical Bonds -- Analysis ; Copper Compounds -- Chemical Properties;
    ISSN: 00201669
    E-ISSN: 1520-510X
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  • 7
    Language: English
    In: Inorganic Chemistry, Feb 18, 2013, Vol.52(4), pp.1673-1675
    Keywords: Luminescence – Analysis ; Boron Compounds – Electric Properties ; Zinc Compounds – Electric Properties
    ISSN: 0020-1669
    Source: Cengage Learning, Inc.
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  • 8
    Language: English
    In: Inorganic chemistry, 04 August 2014, Vol.53(15), pp.8036-44
    Description: Four BMes2Ar (Mes = mesityl, Ar = phenyl or duryl) functionalized 1,3-diketonato ligands have been investigated for use in selective sensitization of Tb(III) and Eu(III) emission. These ligands have the general formula of [R1C(O)CR2C(O)R3](-) (R1 = Ph, R2 = H, R3 = p-Ph-BMes2, L1; R1 = R3 = p-Ph-BMes2, R2 = H, L2; R1 = R3 = Me, R2 = p-Ph-BMes2, L3; R1 = R3 = Me, R2 = p-duryl-BMes2, L4) and belong to class I (L1 and L2) and class II (L3 and L4), respectively. In class I, the boron unit is conjugated with the phenyl linker and the diketone backbone, while in class II, the boron unit, the linker unit, and the diketone unit are nonconjugated with a mutually orthogonal arrangement. To understand the impact of the location of the BMes2Ar unit on the electronic properties of the 1,3-diketone molecules and their ability in activating lanthanide emission, the difluoroboron chelate compounds (1-BF2 to 4-BF2) of ligands L1-L4 were synthesized and examined. The class I ligands were effective in activating Eu(III) emission, while the class II ligands were effective in activating Tb(III) emission. Four Ln(III) complexes, 1Eu, 2Eu, 3Tb, and 4Tb, based on the L1-L4 ligands, respectively, were prepared and examined. The emission quantum efficiency of 1Eu and 2Eu is low (Φ(Eu) ≤ 0.01 in THF, 0.07-0.13 in the solid state), but can be greatly enhanced by the addition of fluoride ions. In contrast, the complex 4Tb has a moderate emission efficiency (Φ(Tb) = 0.14 in THF, 0.47 in the solid state) and experiences a distinct emission quenching upon the addition of fluoride. The selective sensitization of Eu(III) and Tb(III) by L1-L4 and the distinct luminescent response of their Ln(III) complexes toward fluoride ions are caused by the distinct intraligand charge transfer transitions of the two different classes of ligands involving the BMes2 unit.
    Keywords: Terbium -- Electric Properties ; Europium -- Electric Properties ; Emission Spectra -- Analysis;
    ISSN: 00201669
    E-ISSN: 1520-510X
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  • 9
    Language: English
    In: Inorganic chemistry, 18 February 2013, Vol.52(4), pp.1673-5
    Description: A luminescent triarylboron ligand functionalized with three carboxylic groups has been synthesized and fully characterized. Its use in boron-containing metal-organic frameworks (B-MOFs) has been demonstrated by the synthesis and isolation of a Zn(II)B-MOF compound (B-MOF-1). The crystals of B-MOF-1 belong to the cubic space group F432 with 8-fold interpenetrated networks and ∼21% void space. B-MOF-1 exhibits blue fluorescence and is capable of modest gas sorption of N(2), argon, and CO(2).
    Keywords: Luminescence ; Boron Compounds -- Chemistry ; Carboxylic Acids -- Chemistry ; Organometallic Compounds -- Chemistry ; Zinc -- Chemistry
    ISSN: 00201669
    E-ISSN: 1520-510X
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  • 10
    Language: English
    In: Inorganic chemistry, 16 July 2018, Vol.57(14), pp.8581-8587
    Description: The use of a new second-sphere coordination methodology for emission color tuning of iridium complexes is presented. We demonstrate that a complementary H-bonding guest molecule binding through contiguous triple H-bonding interactions can induce a shift in the emission of the iridium complex from green to blue without the need to alter the ligand structure around the metal center, while simultaneously increasing the photoluminescence quantum yield in solution. The association constant for this host-guest interaction was determined to be K = 4.3 × 10 M in a solution of 2% dimethyl sulfoxide in chloroform by UV-vis titration analysis and the impact of the hydrogen bonding interaction further probed by photoluminescence, electrochemical, and computational methods. Our findings suggest that directed self-assemblies are an effective approach to influencing emission properties of phosphorescent iridium(III) complexes.
    ISSN: 00201669
    E-ISSN: 1520-510X
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