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Cobalt-Catalyzed Enantioselective Reductive Coupling of Imines and Internal Alkynes.
Angew Chem Int Ed Engl
January 2025
IISER Kolkata: Indian Institute of Science Education and Research Kolkata, Department of Chemical Sciences, Mohanpur, 741246, Nadia, INDIA.
Chiral allyl amines are important structural components in natural products, pharmaceuticals, and chiral catalysts. Herein, we report a cobalt-catalyzed enantioselective reductive coupling of imines with internal alkynes to synthesize chiral allyl amines. The reaction is catalyzed by a cobalt complex derived from commercially available bisphosphine ligand utilizing zinc as the electron donor.
View Article and Find Full Text PDFCobalt Complexes with Aminophenolate Ligands: Spin Crossover and Ligand Versatility.
Inorg Chem
January 2025
School of Chemistry, University of Melbourne, Parkville 3010, Victoria, Australia.
A search for switchable molecules has afforded a family of cobalt complexes featuring derivatives of 2-aminophenol: 4,6-di--butyl aminophenol (HL) and 2-anilino-4,6-di--butyl aminophenol (HL). The heteroleptic cobalt complexes incorporate a Metpa ligand (tpa = tris(2-pyridylmethyl)amine; = 0-3), which involves the methylation of the 6-position of the pyridine ring). Eight members of this family have been synthesized and characterized: [Co(HL)(tpa)](BPh) (), [Co(HL)(Metpa)](BPh) (), [Co(L)(Metpa)](BPh) (), [Co(HL)(Metpa)](BPh) (), [Co(L)(Metpa)](BPh) (), [Co(HL)(tpa)] (BPh)(ClO) (), [Co(L)(tpa)](BPh)(ClO) () and [Co(HL)(Metpa)](BPh) (), where the aminophenol-derived ligands are monoanionic in either the open shell radical iminosemiquinonate (L) or the closed shell protonated aminophenolate (HL).
View Article and Find Full Text PDFMultifunctional Supramolecular Gels with Strong Mechanical Properties Formed by Self-Assembly of Polyoxometalate-Based Coordination Polymers.
JACS Au
December 2024
Sorbonne Université, CNRS, Institut Parisien de Chimie Moléculaire, IPCM, F-75005 Paris, France.
Metallogels built in a bottom-up approach by metal coordination and supramolecular interactions have important potential for the elaboration of smart materials. In this context, we present here the formation of supramolecular coordination polymers driven by the complexation of cobalt(II) or zinc(II) ions with polyoxometalate-based hybrids displaying two terpyridine ligands in a linear arrangement. Thanks to the electrostatic interactions between the polyoxometalate cores and metal nodes, the polymer chains self-assemble into fibers that physically cross-link to form gels above a critical concentration.
View Article and Find Full Text PDFForce-Activated Spin-Crossover in Fe and Co Transition Metal Mechanophores.
Inorg Chem
December 2024
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139, United States.
Transition metal mechanophores exhibiting force-activated spin-crossover are attractive design targets, yet large-scale discovery of them has not been pursued due in large part to the time-consuming nature of trial-and-error experiments. Instead, we leverage density functional theory (DFT) and external force explicitly included (EFEI) modeling to study a set of 395 feasible Fe and Co mechanophore candidates with tridentate ligands that we curate from the Cambridge Structural Database. Among nitrogen-coordinating low-spin complexes, we observe the prevalence of spin crossover at moderate force, and we identify 155 Fe and Co spin-crossover mechanophores and derive their threshold force for low-spin to high-spin transition ().
View Article and Find Full Text PDFExperimental Spin State Determination of Iron(II) Complexes by Hirshfeld Atom Refinement.
Chemistry
December 2024
Institute of Inorganic Chemistry, RWTH Aachen University, Landoltweg 1a, 52074, Aachen, Germany.
In this study, we present the first experimental determination of the spin state of transition metal complexes by using Hirshfeld Atom Refinement. For the demonstration, the two iron(II) complexes, (NH)Fe(SO) ⋅ 6 HO and lFe(pic)jCl ⋅ EtOH were investigated. The method involves the refinement using wavefunctions of different spin multiplicity and comparison against experimental diffraction data by means of refinement indicators and residual electron density.
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