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Structural Snapshots of Reversible Carbon Dioxide Capture and (De)oxygenation at Group 14 Diradicaloids.
J Am Chem Soc
December 2024
Molecular Inorganic Chemistry and Catalysis, Inorganic and Structural Chemistry, Center for Molecular Materials, Faculty of Chemistry, Universität Bielefeld, Universitätsstrasse 25, D-33615 Bielefeld, Germany.
Article Synopsis
- The study investigates the activation and functionalization of carbon dioxide using stable Group 14 diradicals, specifically focusing on anionic dicarbene frameworks.
- These diradicaloids react with CO to form various compounds through cycloaddition, with behaviors varying significantly depending on the element (Si, Ge, Sn) present in the diradical structure.
- The research includes detailed molecular analysis through X-ray diffraction and theoretical insights from DFT calculations to understand the mechanisms involved in the formation of these compounds.
Direct observation of β-alkynyl eliminations from unstrained propargylic alkoxide Cu(i) complexes by C-C bond cleavage.
Chem Sci
September 2024
Institute for Integrated Catalysis, Pacific Northwest National Laboratory Richland WA 99352 USA
β-Carbon eliminations of aryl, allylic, and propargylic alkoxides of Rh(i), Pd(ii), and Cu(i) are key elementary reactions in the proposed mechanisms of homogeneously catalysed cross-coupling, group transfer, and annulation. Besides the handful of studies with isolable Rh(i)-alkoxides, β-carbon eliminations of Pd(ii)- and Cu(i)-alkoxides are less definitive. Herein, we provide a comprehensive synthetic, structural, and mechanistic study on the β-alkynyl eliminations of isolable secondary and tertiary propargylic alkoxide Cu(i) complexes, LCuOC(H)(Ph)C[triple bond, length as m-dash]CPh and LCuOC(Ar)C[triple bond, length as m-dash]CPh (L = N-heterocyclic carbene (NHC), dppf, -BINAP), to produce monomeric (NHC)CuC[triple bond, length as m-dash]CPh, dimeric [(diphosphine)CuC[triple bond, length as m-dash]CPh], and the corresponding carbonyl.
View Article and Find Full Text PDFPhotosystem I complexes form remarkably stable self-assembled tunneling junctions.
Nanoscale
October 2024
Stratingh Institute for Chemistry, University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands.
This paper describes large-area molecular tunneling junctions comprising self-assembled monolayers (SAMs) of light-harvesting protein complexes using eutectic Ga-In (EGaIn) as a top contact. The complexes, which are readily isolable in large quantities from spinach leaves, self-assemble on top of SAMs of [6,6]-phenyl-C-butyric acid (PCBA) on gold (Au) supported by mica substrates (Au), which induces them to adopt a preferred orientation with respect to the electron transport chain that runs across the short axis of each complex, leading to temperature-independent rectification. We compared trimeric protein complexes isolated from thermophilic cyanobacteria to monomeric complexes extracted from spinach leaves by measuring charge-transport at variable temperatures and over the course of at least three months.
View Article and Find Full Text PDFOrganomagnesia: Reversibly High Carbon Dioxide Uptake by Magnesium Pyrazolates.
Adv Sci (Weinh)
August 2024
Institut für Anorganische Chemie, Eberhard Karls Universität Tübingen, Auf der Morgenstelle 18, 72076, Tübingen, Germany.
A series of new pyrazolate and mixed pyrazolate/pyrazole magnesium complexes is described and their reactivity toward carbon dioxide is examined. The dimeric complex [Mg(pz )] inserts CO instantly and quantitatively forming the tetrameric complex [Mg(CO·pz )] and monomeric donor-stabilized [Mg(CO·pz )(thf)]. Complexes of the type [Mg(pz) (Hpz)] (R = iPr, tBu) engage in similar insertion reactions involving dissociation of the carbamic acid HOOCpz.
View Article and Find Full Text PDFStrain-Induced Structural Rearrangement Towards a White-Light-Emitting Adamantane-Type Cluster Dimer.
Angew Chem Int Ed Engl
December 2024
Institute of Nanotechnology, Karlsruhe Institute of Technology, Kaiserstrasse 12, 76131, Karlsruhe, Germany.
Group 14/16 adamantane-type hybrid clusters of the type [(RT)E] (T=group 14 element, E=group 16 element, R=organic group) have been reported to emit white-light when irradiated in an amorphous state with a continuous-wave (CW) infrared laser diode. This effect is enhanced if the cluster core is varied from a binary to a more complex composition. To further explore this phenomenon, we synthesized clusters with a multinary R/R'-T/T'-E/E' composition, including isolobal replacement of E with CH, in [(2-NpSi){CHSn(S)Ph}] (1, Np=naphthyl).
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