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The synthesis and characterization of carboxylate-bridged dimetallic complexes are described. By using m-terphenyl-derived carboxylate ligands, a series of dicobalt(II), dicobalt(III), dinickel(II), and dizinc(II) complexes were synthesized. The compounds are [Co(2)(mu-O(2)CAr(Tol))(2)(O(2)CAr(Tol))(2)L(2)] (1), [Co(2)(mu-OH(2))(2)(mu-O(2)CAr(Tol))(2)(O(2)CAr(Tol))(2)L(2)] (2a-c), [Co(2)(mu-OH)(2)(mu-O(2)CAr(Tol))(2)(O(2)CAr(Tol))(2)L(2)] (3), [Ni(2)(mu-O(2)CAr(Tol))(4)L(2)] (4), [Ni(2)(mu-HO...

ADVERTISEMENT RETURN TO ISSUEPREVCommunicationNEXTStructural and Functional Models of the Dioxygen-Activating Centers of Non-Heme Diiron Enzymes Ribonucleotide Reductase and Soluble Methane MonooxygenaseDongwhan Lee and Stephen J. LippardView Author Information Department of Chemistry Massachusetts Institute of Technology Cambridge, Massachusetts 02139 Cite this: J. Am. Chem. Soc. 1998, 120, 46, 12153–12154Publication Date (Web):November 10, 1998Publication History Received31 August 1998Publishe

ADVERTISEMENT RETURN TO ISSUEPREVCommunicationNEXTFormation of Fe(III)Fe(IV) Species from the Reaction between a Diiron(II) Complex and Dioxygen: Relevance to Ribonucleotide Reductase Intermediate XDongwhan Lee, J. Du Bois, Doros Petasis, Michael P. Hendrich, Carsten Krebs, Boi Hanh Huynh, and Stephen J. LippardView Author Information Department of Chemistry Massachusetts Institute of Technology Cambridge, Massachusetts 02139 Department of Chemistry, Carnegie Mellon University Pittsburgh, Pennsy

ADVERTISEMENT RETURN TO ISSUEPREVCommunicationNEXTOxidative N-Dealkylation of a Carboxylate-Bridged Diiron(II) Precursor Complex by Reaction with O2 Affords the Elusive {Fe2(μ-OH)2(μ-O2CR)}3+ Core of Soluble Methane Monooxygenase HydroxylaseDongwhan Lee and Stephen J. LippardView Author Information Department of Chemistry Massachusetts Institute of Technology Cambridge, Massachusetts 02139 Cite this: J. Am. Chem. Soc. 2001, 123, 19, 4611–4612Publication Date (Web):April 18, 2001Publication Histo

A canopy-shaped pyrrole derivative 2 was prepared, in which a sterically demanding pendant group is juxtaposed to the pyrrole fragment to minimize interstrand pi-pi stacking interactions in the resulting polymer. Anodic polymerization of 2 afforded highly conductive poly(2), the electronic structure of which was probed by various spectroelectrochemical techniques. A limited charge delocalization within poly(2) translates into a well-defined conductivity profile, properties important for resistiv

General synthetic routes are described for a series of diiron(II) complexes supported by sterically demanding carboxylate ligands 2,6-di(p-tolyl)benzoate (Ar(Tol)CO(2)(-)) and 2,6-di(4-fluorophenyl)benzoate (Ar(4-FPh)CO(2)(-)). The interlocking nature of the m-terphenyl units in self-assembled [Fe(2)(mu-O(2)CAr(Tol))(2)(O(2)CAr(Tol))(2)L(2)] (L = C(5)H(5)N (4); 1-MeIm (5)) promotes the formation of coordination geometries analogous to those of the non-heme diiron cores in the enzymes RNR-R2 and

ADVERTISEMENT RETURN TO ISSUEPREVCommunicationNEXTValence-Delocalized Diiron(II,III) Cores Supported by Carboxylate-Only Bridging LigandsDongwhan Lee, Carsten Krebs, Boi Hanh Huynh, Michael P. Hendrich, and Stephen J. LippardView Author Information Department of Chemistry Massachusetts Institute of Technology Cambridge, Massachusetts 02139 Department of Physics, Emory University Atlanta, Georgia 30322 Department of Chemistry, Carnegie Mellon University Pittsburgh, Pennsylvania 15213 Cite this: J

A new bipolar-type redox-active organic material with a wide HOMO–LUMO energy gap is designed though the ‘p–n fusion’ strategy.

Two tetracarboxylate diiron(II) complexes, [Fe(2)(mu-O(2)CAr(Tol))(2)(O(2)CAr(Tol))(2)(C(5)H(5)N)(2)] (1a) and [Fe(2)(mu-O(2)CAr(Tol))(4)(4-(t)BuC(5)H(4)N)(2)] (2a), where Ar(Tol)CO(2)(-) = 2,6-di(p-tolyl)benzoate, react with O(2) in CH(2)Cl(2) at -78 degrees C to afford dark green intermediates 1b (lambda(max) congruent with 660 nm; epsilon = 1600 M(-1) cm(-1)) and 2b (lambda(max) congruent with 670 nm; epsilon = 1700 M(-1) cm(-1)), respectively. Upon warming to room temperature, the solutions

A series of air-stable boron complexes 1-5 were prepared by using N-aryl iminopyrrolide ligands. Designed as minimalist structural mimics of the privileged BODIPY motif, these new BOIMPY (BOron complexes of IMinoPYrrolide ligands) fluorophores feature low molecular symmetry that promotes emission from CT-type excited states with large Stokes shifts and little self-quenching. Through comparative studies on the homologous set of compounds 1-4, we have confirmed that a delicate interplay between co

We describe the synthesis and dioxygen reactivity of diiron(II) tetracarboxylate complexes [Fe(2)(mu-O(2)CAr(Tol))(2)(O(2)CAr(Tol))(2)(N,N-Me(2)en)(2)] (2) and [Fe(2)(mu-O(2)CAr(Tol))(2)(O(2)CAr(Tol))(2)(N,N-Bn(2)en)(2)] (6), where Ar(Tol)CO(2)(-) = 2,6-di(p-tolyl)benzoate. These complexes were prepared as models for the diiron(II) center in the hydroxylase component of soluble methane monooxygenase (MMOH). Compound 6 reacts with dioxygen to afford PhCHO in approximately 60(5)% yield, following

The development of white-light-emitting polymers has been actively pursued because of the importance of such polymers in various applications, such as lighting sources and displays. To generate white-light, numerous research efforts have focused on synthesizing multifluorophore-based random copolymers to effectively cover the entire visible region. However, due to their intrinsic synthetic and structural features, this strategy has limitations in securing color reproducibility and stability. Her

Entry into a new class of tetra- and dicopper clusters was assisted by a fine steric tuning of bulky amidinate ligands that provide spin-delocalizing superexchange pathways in class III mixed-valence clusters, the properties of which are best understood without invoking metal-metal bonding.

The design, synthesis, and electropolymerization of sterically hindered pyrrole derivatives are described. Endo and exo adducts of cyclopentadiene and N-phenylmaleimide were converted to give bicyclo[2.2.1]heptane-fused pyrrole monomers, in which a phenyl group is rigidly placed proximate the pyrrole fragment. Oxidative polymerization of these monomers affords highly conductive polypyrroles. The rigid molecular scafffold of the pyrrole monomers limits cross-communication between adjacent conduct

Small molecule self-assembly at surfaces offers an efficient route to highly ordered organic films that can be programmed for a variety of chemical and electronic applications. The success of these materials depends on the ability to program intermolecular interactions to guide precise structural ordering. Toward this objective, we have designed and synthesized a series of bis(triazolo)benzene-based π-conjugated molecules. Our synthesis exploits a last-stage C-C cross-coupling reaction to close