Fischer carbene complex anchored on glass or silicon surface using a Cu-free 'click' reaction allows facile and swift covalent grafting of protein molecules like Bovine Serum Albumin (BSA).
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A Discrete Trialane with a Near-Linear Al Axis.
J Am Chem Soc
December 2024
Institute for Inorganic Chemistry, Julius-Maximilians-Universität Würzburg, Am Hubland, 97074 Würzburg. Germany.
The presence of inherent electronic unsaturation in aluminum predominantly results in the formation of aluminum clusters, with very few examples of compounds containing discrete chains of aluminum atoms in existence. In this work, we present the successful synthesis and structural authentication of a highly unusual trialane species with a near-linear chain of three Al atoms, alongside a carbene-stabilized aluminyl anion ([LAlR]), an alternative product produced by varying the reaction conditions. Quantum-chemical calculations have been applied to elucidate the electronic structure and bonding of these novel compounds.
View Article and Find Full Text PDFRing-Opening Metathesis Polymerization of 1,2-Dihydroazete Derivatives.
Angew Chem Int Ed Engl
November 2024
Department School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia, 30332, United States.
Fischer carbenes have recently found great utility in the construction of degradable metathesis materials, but investigations have been limited to oxygen-containing enol ether monomers. Here, the ring-opening metathesis polymerization of 1,2-dihydroazetes is reported. The polymerization proceeds regioselectively, and the resulting molecular weights are targetable by adjusting the Grubbs initiator loading.
View Article and Find Full Text PDFThe Tetrafluoroethylene-Mediated Ring-Closing Metathesis: Enabling Unfavored Reactions.
J Am Chem Soc
November 2024
Department of Chemistry and Biotechnology, Graduate School of Engineering, The University of Tokyo, Tokyo 113-0032, Japan.
While ring-closing metathesis (RCM) is a powerful method for constructing medium and large cyclic alkenes, its application to the synthesis of heterocycles faces considerable limitations. For instance, RCM of divinyloxyalkanes does not proceed under the conventional conditions of RCM. The challenge lies in the formation of stable Fischer-type carbene intermediates with heteroatom(s) bound to the carbene carbon, impeding subsequent metathesis.
View Article and Find Full Text PDFHeavier Diferrocenylpnictogenium Ions.
Chemistry
October 2024
Institut für Anorganische Chemie und Kristallographie, Universität Bremen, Leobener Straße 7, 28359, Bremen, Germany.
The synthesis, characterization and reactivity of the diferrocenylphosphenium ion [FcP] was extended to the heavier diferrocenylpnictogenium ions, [FcE] (E=As, Sb, Bi). The lighter diferrocenylnitrenium ion, [FcN], was detected by mass spectrometry, but could not be isolated. The molecular structures of [FcE] (E=P, As, Sb, Bi) reveal intramolecular coordination of the iron atoms, which counterbalance the electron deficiency of the pnictogens without affecting the strong Lewis acidities, which were determined according to the method of Gutmann and Beckett.
View Article and Find Full Text PDFC-H Insertion from Isolable Copper Benzylidenes.
J Am Chem Soc
November 2024
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, United States.
Despite the utility of copper catalysts for the insertion of carbene moieties into C-H bonds, the copper carbene intermediate often invoked in these transformations has not been isolated. Herein, we describe the synthesis and structural characterization of a series of copper benzylidenes utilizing the sterically encumbered dipyrrin ligand (L)H. These isolated copper carbenes demonstrate intramolecular insertion into the primary C(sp)-H bond of the ligand (L)H and intermolecular insertion into ethereal and allylic C-H bonds.
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