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Themed collection Bioinspired metal complexes for chemical transformations and catalysis

21 items
Accepted Manuscript - Feature Article

Bioinspired metal complexes for energy-related photocatalytic small molecule transformation

Communication

Bridging and axial carbene binding modes in cobalt corrole complexes: effect on carbene transfer

Two different types of carbene intermediates are observed in the reaction of ethyl diazoacetate (EDA) with different Co corrole complexes, and their properties and reactivities are reported.

Graphical abstract: Bridging and axial carbene binding modes in cobalt corrole complexes: effect on carbene transfer
Open Access Communication

Ambiphilicity of a mononuclear cobalt(III) superoxo complex

Addition of HOTf to a mixture of CoIII(BDPP)(O2˙) (1) and Cp*2Fe produced H2O2 in high yield implying formation of CoIII(BDPP)(OOH) (3), and reaction of Sc(OTf)3 with the same mixture gave a peroxo-bridged CoIII/ScIII5.

Graphical abstract: Ambiphilicity of a mononuclear cobalt(iii) superoxo complex
Communication

Catalytic O2 activation with synthetic models of α-ketoglutarate dependent oxygenases

An iron complex with a tridentate 1,4,7-triazacyclononane ligand mimics structural and functional features of α-ketoglutarate (α-KG) dependent enzymes, and engages in catalytic O2 activation coupled to α-KG decarboxylation and sulfide oxygenation.

Graphical abstract: Catalytic O2 activation with synthetic models of α-ketoglutarate dependent oxygenases
Communication

Revisiting amorphous molybdenum sulfide's activity for the electro-driven reduction of dinitrogen and N-containing substrates

Amorphous molybdenum sulfide exhibits partial nitrogenase-like activity allowing for the electro driven reduction of azides under aqueous conditions.

Graphical abstract: Revisiting amorphous molybdenum sulfide's activity for the electro-driven reduction of dinitrogen and N-containing substrates
Communication

Mobility of Lewis acids within the secondary coordination sphere: toward a model for cooperative substrate binding

Distance dependence of appended Lewis acids in N2H4 binding and deprotonation was evaluated within a series of zinc complexes.

Graphical abstract: Mobility of Lewis acids within the secondary coordination sphere: toward a model for cooperative substrate binding
Communication

Ligand regulation for manganese-catalyzed enantioselective epoxidation of olefins without acid

A manganese-catalyzed asymmetric epoxidation of olefins is developed under acid-free conditions. MnIV[double bond, length as m-dash]O species serves as an active species.

Graphical abstract: Ligand regulation for manganese-catalyzed enantioselective epoxidation of olefins without acid
Communication

Kinetic and mechanistic analysis of a synthetic reversible CO2/HCO2 electrocatalyst

A kinetic and mechanistic analysis of [Pt(depe)2](PF6)2, an electrocatalyst for the reversible conversion between CO2 and HCO2 with high selectivity at low overpotentials.

Graphical abstract: Kinetic and mechanistic analysis of a synthetic reversible CO2/HCO2− electrocatalyst
Open Access Communication

Copper arylnitrene intermediates: formation, structure and reactivity

The mechanism of oxidation of arylamines by copper enzymes is not clarified yet. A possible pathway involves copper(II)oxyl intermediates transforming arylamines to copper aryl nitrenes. We investigate details of this pathway in a gas phase reaction.

Graphical abstract: Copper arylnitrene intermediates: formation, structure and reactivity
Communication

Spin-resolved charge displacement analysis as an intuitive tool for the evaluation of cPCET and HAT scenarios

The spin-resolved version of the charge displacement function is introduced as an intuitive tool for differentiating between hydrogen-atom transfer and concerted proton-coupled electron transfer.

Graphical abstract: Spin-resolved charge displacement analysis as an intuitive tool for the evaluation of cPCET and HAT scenarios
Communication

Synthesis of a B12–BODIPY dyad for B12-inspired photochemical transformations of a trichloromethylated organic compound

A B12 complex–BODIPY dyad was synthesized by peripheral modification of cobalamin derivatives.

Graphical abstract: Synthesis of a B12–BODIPY dyad for B12-inspired photochemical transformations of a trichloromethylated organic compound
Communication

A NiRhS fuel cell catalyst – lessons from hydrogenase

Novel dry-distilled catalysts based on Rh, Ni and S were developed via a Ni(μ-S)2Rh organometallic [NiFe]hydrogenase mimic.

Graphical abstract: A NiRhS fuel cell catalyst – lessons from hydrogenase
Communication

A heterogeneous bio-inspired peroxide shunt for catalytic oxidation of organic molecules

Iron porphyrins with three different axial ligands installed atop self-assembled monolayer modified gold electrodes can oxidize C–H bonds and epoxidize alkenes efficiently using H2O2via the formation of a high-valent intermediate.

Graphical abstract: A heterogeneous bio-inspired peroxide shunt for catalytic oxidation of organic molecules
Communication

Proton-promoted disproportionation of iron(V)-imido TAML to iron(V)-imido TAML cation radical and iron(IV) TAML

An iron(V)-imido TAML complex is disproportionated to give an iron(V)-imido TAML cation radical and an iron(IV) TAML upon addition of acids.

Graphical abstract: Proton-promoted disproportionation of iron(v)-imido TAML to iron(v)-imido TAML cation radical and iron(iv) TAML
Communication

Bimetallic iron–tin catalyst for N2 to NH3 and a silyldiazenido model intermediate

A new tin-supported iron complex catalyzes N2 fixation. The role of this heavy main group element in the catalysis is evaluated.

Graphical abstract: Bimetallic iron–tin catalyst for N2 to NH3 and a silyldiazenido model intermediate
Communication

Selective catalytic 2e-oxidation of organic substrates by an FeII complex having an N-heterocyclic carbene ligand in water

An FeII complex, 1, having a pentadentate ligand with an NHC moiety catalyzes substrate oxidation to afford 2e-oxidized products with high selectivity by suppression of overoxidation in water.

Graphical abstract: Selective catalytic 2e−-oxidation of organic substrates by an FeII complex having an N-heterocyclic carbene ligand in water
Communication

Controlled O2 reduction at a mixed-valent (II,I) Cu2S core

Oxygen reduction reactions catalyzed by a mixed-valent copper complex reveal a tuneable H2O2/H2O selectivity at room temperature together with high stability over several cycles.

Graphical abstract: Controlled O2 reduction at a mixed-valent (II,I) Cu2S core
Communication

Nucleophilic reactivity of a mononuclear cobalt(III)–bis(tert-butylperoxo) complex

A mononuclear cobalt(III)–bis(tert-butylperoxo) adduct (CoIII–(OOtBu)2) bearing a tetraazamacrocyclic ligand was synthesized and characterized using various physicochemical methods, such as X-ray, UV-vis, ESI-MS, EPR, and NMR analyses.

Graphical abstract: Nucleophilic reactivity of a mononuclear cobalt(iii)–bis(tert-butylperoxo) complex
Communication

Metal–ligand cooperativity across two sites of a square planar iron(II) complex ligated by a tetradentate PNNP ligand

A square planar (PNNP)FeII complex is shown to readily activate two B–H bonds across the Fe–amide linkages in an overall four-electron process facilitated by metal–ligand cooperativity.

Graphical abstract: Metal–ligand cooperativity across two sites of a square planar iron(ii) complex ligated by a tetradentate PNNP ligand
Communication

A dinuclear Mo2H8 complex supported by bulky C5H2tBu3 ligands

A simple dinuclear hydride complex consisting of only Mo, hydrides, and cyclopentadienyl ligands was synthesized and tested for benzene activation.

Graphical abstract: A dinuclear Mo2H8 complex supported by bulky C5H2tBu3 ligands
Communication

Preparation and reactivity of molybdenum complexes bearing pyrrole-based PNP-type pincer ligand

Molybdenum complexes bearing an anionic pyrrole-based PNP-type pincer ligand have been prepared and have been found to work as catalysts for the conversion of N2 into NH3 under ambient conditions.

Graphical abstract: Preparation and reactivity of molybdenum complexes bearing pyrrole-based PNP-type pincer ligand
21 items

About this collection

Designing catalysts that transform small molecules with minimal energy cost while maximizing activity, selectivity, and sustainability is a long-standing challenge. The study of bioinspired metal complexes and metalloenzymes offers new opportunities to move this field forward, whether it is the discovery of a more efficient catalyst, elucidation of a new mechanism, or bringing current interdisciplinary tools to bear.
This Themed Collection, Guest Edited by Connie Lu (University of Minnesota, USA), Liang Deng (Shanghai Institute of Organic Chemistry, CAS, China) and Carole Duboc (University of Grenoble Alpes/CNRS, France) will highlight important on-going work to develop and to understand the structural and/or functional models of metalloenzyme active sites for chemical transformations and catalysis. The metal systems will range from molecular, supramolecular, to more complex networks, such as proteins and metal-organic frameworks.

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