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  • Angewandte Chemie International Edition
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  • 1
    Language: English
    In: Angewandte Chemie International Edition, 08 August 2016, Vol.55(33), pp.9719-9722
    Description: A synthetic approach to dihydropyrrolizine and tetrahydroindolizine scaffolds from pyrroles has been developed. The key step, a titanocene(III)‐catalyzed radical arylation that proceeds by C−H functionalization is atom‐economical and tolerates a large variety of functional groups. The reaction is therefore attractive for the swift assembly of functional and structural diversity. : The catalytic formation of dihydropyrrolizines and tetrahydroindolizines through titanocene(III) catalysis is described. The radical reaction is atom‐economical, tolerates a large variety of functional groups, and proceeds with regioselectivity. It is therefore of interest for applications in the synthesis of biologically active compounds.
    Keywords: Electron Transfer ; Heterocyles ; Radicals ; Reaction Mechanisms ; Titanium
    ISSN: 1433-7851
    E-ISSN: 1521-3773
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  • 2
    Article
    Article
    Language: English
    In: Angewandte Chemie International Edition, 21 June 2010, Vol.49(27), pp.4540-4541
    Description: : A novel application of Raman microscopy takes advantage of a spectral window to map the uptake and distribution of metal‐carbonyl‐based drugs in single cells. The approach provides information on cell structure and molecular structure simultaneously and may have significant impact on drug screening and on the analysis of cellular processes in general.
    Keywords: Antitumor Agents ; Carbonyl Ligands ; Cells ; Molecular Imaging ; Raman Microscopy
    ISSN: 1433-7851
    E-ISSN: 1521-3773
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  • 3
    Language: English
    In: Angewandte Chemie International Edition, 17 August 2015, Vol.54(34), pp.10024-10029
    Description: The importance of microRNA (miRNA) dysregulation for the development and progression of diseases and the discovery of stable miRNAs in peripheral blood have made these short‐sequence nucleic acids next‐generation biomarkers. Here we present a fully homogeneous multiplexed miRNA FRET assay that combines careful biophotonic design with various RNA hybridization and ligation steps. The single‐step, single‐temperature, and amplification‐free assay provides a unique combination of performance parameters compared to state‐of‐the‐art miRNA detection technologies. Precise multiplexed quantification of miRNA‐20a, ‐20b, and ‐21 at concentrations between 0.05 and 0.5 n in a single 150 μL sample and detection limits between 0.2 and 0.9 n in 7.5 μL serum samples demonstrate the feasibility of both high‐throughput and point‐of‐care clinical diagnostics. : An amplification‐free homogeneous “mix‐and‐measure” assay for the multiplexed detection of up to three microRNAs has been developed. It uses Förster resonance energy transfer from a Tb complex donor to three different dye acceptors and is conducted in one step and at a single temperature.
    Keywords: Clinical Diagnostics ; Fret ; Microrna ; Multiplexing ; Time‐Gated Fluorescence Detection
    ISSN: 1433-7851
    E-ISSN: 1521-3773
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  • 4
    Language: English
    In: Angewandte Chemie International Edition, 06 August 2012, Vol.51(32), pp.8114-8117
    Description: : Tethered bilayer lipid membranes containing the cation‐channel‐forming peptide gramicidin A were assembled on nanostructured Au films. The combination of surface‐enhanced infrared absorption (SEIRA) and electrochemical impedance spectroscopy (EIS) was used for the in situ structural and functional characterization of gramicidin A in the same device.
    Keywords: Bilayer Lipid Membranes ; Electrochemistry ; Gramicidin A ; Ion Channels ; Seira
    ISSN: 1433-7851
    E-ISSN: 1521-3773
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  • 5
    Language: English
    In: Angewandte Chemie (International ed. in English), 07 March 2011, Vol.50(11), pp.2632-4
    Description: Includes references ; p. 2632-2634.
    Keywords: Hydrogenase -- Chemistry
    ISSN: 14337851
    E-ISSN: 1521-3773
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  • 6
    Language: English
    In: Angewandte Chemie International Edition, 08/17/2015, Vol.54(34), pp.9725-9725
    Description: The simple, sensitive, and selective detection of short‐sequence microRNAs is very challenging. In their Communication on page 10024 ff. N. Hildebrandt and co‐workers present a single‐step “mix‐and‐measure” FRET assay for the multiplexed detection of different microRNAs. The careful design of the biophotonic probe and time‐gated FRET from a luminescent Tb complex to three difference fluorescent dyes are crucial to this microRNA test for multiplexed clinical diagnostics.
    Keywords: Chemistry;
    ISSN: Angewandte Chemie International Edition
    E-ISSN: 14337851
    E-ISSN: 15213773
    Source: Wiley (via CrossRef)
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  • 7
    Language: English
    In: Angewandte Chemie International Edition, 24 February 2014, Vol.53(9), pp.2481-2484
    Description: Mesoporous M‐TiO NCs, functionalized by PATP, can capture toxic anilines and phenols by azo coupling. Loading these nanodevices with Ag NPs offers the possibility for a sensitive quantitative determination of target compounds by SERRS spectroscopy, which allows multiplex detection because of the specific vibrational fingerprints. Sensitivity and selectivity can be further enhanced by concentrating the hybrid particles by an external magnet and compound‐specific binding (anilines versus phenols). The bound toxic compounds can be degraded by TiO‐assisted photocatalysis after removal of the loaded hybrid particles from the sample solution with an external magnet. The degradation process can be enhanced in the presence of plasmonic Ag nanostructures. (M‐TiO NCs) are fabricated and functionalized for determination and elimination of toxic anilines and phenols. The compounds, bound to M‐TiO NCs by azo coupling, may be degraded by TiO‐assisted photocatalysis, making the NCs recyclable. Addition of Ag nanoparticles allows the detection and identification of the azo products by surface‐enhanced resonance Raman spectroscopy and accelerates photocatalytic detoxification.
    Keywords: Aniline ; Magnetic Tio ; Phenol ; Photocatalysis ; Serrs
    ISSN: 1433-7851
    E-ISSN: 1521-3773
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  • 8
    Language: English
    In: Angewandte Chemie International Edition, 18 November 2011, Vol.50(47), pp.11248-11252
    Description: : Two diferrocenyl‐substituted three‐ and five‐membered titanacycles (see structure) were synthesized. Their molecular structures in the solid state reveal symmetrically arranged metallocene groups connected only by a C or C chain. For the first time, the electrochemical behavior of these systems was studied and a linearization of the ligand in the dication of the five‐membered ring was observed.
    Keywords: Density Functional Calculations ; Electrochemistry ; Heterometallic Complexes ; Metallacycles ; Titanocenes
    ISSN: 1433-7851
    E-ISSN: 1521-3773
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  • 9
    Language: English
    In: Angewandte Chemie International Edition, Jan, 2014, Vol.53(1), p.205(5)
    Description: Byline: Isidoro Lopez, Mehmed Z. Ertem, Somnath Maji, Jordi Benet-Buchholz, Anke Keidel, Uwe Kuhlmann, Peter Hildebrandt, Christopher J. Cramer, Victor S. Batista, Antoni Llobet Keywords: density functional calculations; reaction mechanisms; resonance Raman spectroscopy; ruthenium electrochemistry; water-oxidation catalysis Abstract The homogeneous catalysis of water oxidation by transition-metal complexes has experienced spectacular development over the last five years. Practical energy-conversion schemes, however, require robust catalysts with large turnover frequencies. Herein we introduce a new oxidatively rugged and powerful dinuclear water-oxidation catalyst that is generated by self-assembly from a mononuclear catalyst during the catalytic process. Our kinetic and DFT computational analysis shows that two interconnected catalytic cycles coexist while the mononuclear system is slowly and irreversibly converted into the more stable dinuclear system: an extremely robust water-oxidation catalyst that does not decompose over extended periods of time. Author Affiliation: Institute of Chemical Research of Catalonia (ICIQ), Av. Paisos Catalans 16, 43007 Tarragona (Spain) Technische Universitat Berlin, Institut fur Chemie, Sekr. PC14, Strasse des 17. Juni 135, 10623 Berlin (Germany) Department of Chemistry, Brookhaven National Laboratory, Building 555A, Upton, NY 11973 (USA) Department of Chemistry, Yale University, P.O. Box 208107, New Haven, CT 06520-8107 (USA) Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota, 207 Pleasant Street SE, Minneapolis, MN 55455-0431 (USA) Article Note: Support from MINECO (CTQ2010-21497 and PRI-PIBIN-2011-1278), an FPU grant to I.L., and a Torres Quevedo contract to S.M. are gratefully acknowledged. Support has also been received from the Cluster of Excellence (UniCat) and the US Department of Energy (DOE) (Grant DE-SC0001423 to V.S.B.). M.Z.E. received funding from a Computational Materials and Chemical Sciences (CMCSN) project at Brookhaven National Laboratory under contract DE-AC02-98CH10886 with the US DOE and was supported by its Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences. C.J.C. acknowledges support from the US National Science Foundation (CHE-0952054). Supporting information: Additional Supporting Information may be found in the online version of this article As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. CAPTION(S): miscellaneous_information
    Keywords: Ruthenium -- Analysis ; Oxidation-reduction Reactions -- Analysis ; Raman Spectroscopy -- Analysis ; Platinum Group Compounds -- Analysis ; Electrochemistry -- Analysis ; Electrochemical Reactions -- Analysis
    ISSN: 1433-7851
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  • 10
    Language: English
    In: Angewandte Chemie International Edition, 02 January 2017, Vol.56(1), pp.297-301
    Description: The strikingly different reactivity of a series of homo‐ and heterodinuclear [(M)(μ‐O)(M)′] (M=Ni; M′=Fe, Co, Ni and M=M′=Co) complexes with β‐diketiminate ligands in electrophilic and nucleophilic oxidation reactions is reported, and can be correlated to the spectroscopic features of the [(M)(μ‐O)(M)′] core. In particular, the unprecedented nucleophilic reactivity of the symmetric [Ni(μ‐O)Ni] complex and the decay of the asymmetric [Ni(μ‐O)Co] core through aromatic hydroxylation reactions represent a new domain for high‐valent bis(μ‐oxido)dimetal reactivity. : The decisive effect of the second metal ion on the electronic structure and reactivity (from nucleophilic to electrophilic) of a series of [Ni(μ‐O)M] complexes in oxidation reactions is reported. The observations underline the importance of subtle electronic differences in the reactivity of biologically relevant metal–dioxygen intermediates.
    Keywords: Dioxygen Activation ; Heterobimetallic Complex ; Metal–Oxo Complexes ; Nih Shift ; Nucleophilic Oxidant
    ISSN: 1433-7851
    E-ISSN: 1521-3773
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