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Themed collection Breaking bonds over many timescales: in celebration of Robin Perutz’s 70th birthday

27 items
Editorial

Breaking bonds over many timescales: in celebration of Robin Perutz's 70th birthday

We are delighted to present this collection of articles to celebrate Professor Robin Perutz’s 70th birthday.

Graphical abstract: Breaking bonds over many timescales: in celebration of Robin Perutz's 70th birthday
Perspective

Bonding rearrangements in organometallic reactions: from orbitals to curly arrows

The movement of the center of charge of localized orbitals along a reaction pathway draws the curly arrows describing the bonding rearrangement.

Graphical abstract: Bonding rearrangements in organometallic reactions: from orbitals to curly arrows
Communication

The dilemma between acid and base catalysis in the synthesis of benzimidazole from o-phenylenediamine and carbon dioxide

Synthesis of azoles from ortho-substituted anilines and CO2 is limited by the cyclization reaction and not by CO2 reduction.

Graphical abstract: The dilemma between acid and base catalysis in the synthesis of benzimidazole from o-phenylenediamine and carbon dioxide
From the themed collection: Celebrating our 2020 Prize and Award winners
Communication

CO2 activation by manganese pincer complexes through different modes of metal–ligand cooperation

Activation of CO2 by manganese pincer complexes using two different modes of metal–ligand cooperativity (amido/amino mode and dearomatization/aromatization mode) is reported.

Graphical abstract: CO2 activation by manganese pincer complexes through different modes of metal–ligand cooperation
Communication

Palladium-mediated intramolecular dearomatization of ligated dialkylterphenyl phosphines

Thermal dearomative rearrangement of coordinated dialkylterphenyl phosphines mediated by Pd(II).

Graphical abstract: Palladium-mediated intramolecular dearomatization of ligated dialkylterphenyl phosphines
Communication

The experimental determination of Th(IV)/Th(III) redox potentials in organometallic thorium complexes

ThIV/ThIII reduction wave in the cyclic voltammogram of [Th(η-C5H3{SiMe3}2)3Cl].

Graphical abstract: The experimental determination of Th(iv)/Th(iii) redox potentials in organometallic thorium complexes
Paper

Sterically hindered Re- and Mn-CO2 reduction catalysts for solar energy conversion

M(NN)(CO)3X (M = Re, Mn) complexes with a bulky diimine ligand catalyse electrochemical reduction of CO2 with high TON. A noble-metal free system of the Mn-complex photosensitised by a Zn-porphyrin photocatalytically reduces CO2 under visible light.

Graphical abstract: Sterically hindered Re- and Mn-CO2 reduction catalysts for solar energy conversion
Open Access Paper

Insights from semi-oriented EPR spectroscopy studies into the interaction of lytic polysaccharide monooxygenases with cellulose

Semi-orientated EPR spectroscopy reveals that lytic polysaccharide monooxygenases interact with their natural cellulose substrate in a specific way, where the copper active site is positioned adjacent to the edge of a crystalline cellulose fibril.

Graphical abstract: Insights from semi-oriented EPR spectroscopy studies into the interaction of lytic polysaccharide monooxygenases with cellulose
From the themed collection: Celebrating our 2020 Prize and Award winners
Paper

Organometallic chemistry in aqua regia: metal and ligand based oxidations of (NHC)AuCl complexes

The synthesis and characterization of a series of N-heterocyclic Au(III) carbene complexes prepared by oxidation of (NHC)AuCl in aqua regia is described.

Graphical abstract: Organometallic chemistry in aqua regia: metal and ligand based oxidations of (NHC)AuCl complexes
Open Access Paper

Dicerium letterbox-shaped tetraphenolates: f-block complexes designed for two-electron chemistry

Well-defined dinuclear lanthanide complexes: stabilisation of both CeIII and CeIV.

Graphical abstract: Dicerium letterbox-shaped tetraphenolates: f-block complexes designed for two-electron chemistry
Paper

Reversible photo-isomerization of cis-[Pd(L-κS,O)2] (HL = N,N-diethyl-N′-1-naphthoylthiourea) to trans-[Pd(L-κS,O)2] and the unprecedented formation of trans-[Pd(L-κS,N)2] in solution

Ex-situ with polychromatic or in-situ laser light irradiation of solutions of pure cis-[Pd(L-κS,O)2] leads to the formation of trans-[Pd(L-κS,O)2] species that in the dark reverts via an unprecedented trans-[Pd(L-κS,N)2] cleanly to the cis-[Pd(L-κS,O)2].

Graphical abstract: Reversible photo-isomerization of cis-[Pd(L-κS,O)2] (HL = N,N-diethyl-N′-1-naphthoylthiourea) to trans-[Pd(L-κS,O)2] and the unprecedented formation of trans-[Pd(L-κS,N)2] in solution
Paper

A general benzylic C–H activation and C–C coupling reaction of zirconocenes mediated by C–N bond cleavage in tert-butylisocyanide – unusual formation of iminoacyl complexes

Reactions of the zirconocene alkyne complex [rac-(ebthi)Zr(η2-Me3SiC2SiMe3)] (rac-(ebthi) = rac-1,2-ethylene-1,1′-bis(η5-tetrahydroindenyl)) with tert-butylisocyanide and methylbenzenes were investigated.

Graphical abstract: A general benzylic C–H activation and C–C coupling reaction of zirconocenes mediated by C–N bond cleavage in tert-butylisocyanide – unusual formation of iminoacyl complexes
Paper

Phosphine-free ruthenium NCN-ligand complexes and their use in catalytic CO2 hydrogenation

A ruthenium hydride with a fluxional NHC ligand catalyses the hydrogenation of carbon dioxide.

Graphical abstract: Phosphine-free ruthenium NCN-ligand complexes and their use in catalytic CO2 hydrogenation
Paper

Insight into the mechanism of CO-release from trypto-CORM using ultra-fast spectroscopy and computational chemistry

Photolysis of trypto-CORM results in ultra-fast CO-dissociation and formation of a 16-e triplet followed by solvation.

Graphical abstract: Insight into the mechanism of CO-release from trypto-CORM using ultra-fast spectroscopy and computational chemistry
Paper

C–H and C–F bond activation reactions of pentafluorostyrene at rhodium complexes

Reactions of various Rh(I) complexes towards penta-fluorostyrene or its borylated derivative afforded coordination and C–F bond or C–H bond activation reactions.

Graphical abstract: C–H and C–F bond activation reactions of pentafluorostyrene at rhodium complexes
Paper

A biotin-conjugated photo-activated CO-releasing molecule (biotinCORM): efficient CO-release from an avidin–biotinCORM protein adduct

A biotinylated carbon monoxide-releasing molecule (BiotinCORM) releases CO by photoirradiation at 400 nm; an avidin–biotinCORM adduct is an effective CO-releasing molecule.

Graphical abstract: A biotin-conjugated photo-activated CO-releasing molecule (biotinCORM): efficient CO-release from an avidin–biotinCORM protein adduct
Paper

The diverse mechanisms for the oxidative addition of C–Br bonds to Pd(PR3) and Pd(PR3)2 complexes

The reaction between bromobenzene and palladium(0) complexes leading to a palladium(II) complex containing bromide and phenyl ligands is studied computationally with DFT methods.

Graphical abstract: The diverse mechanisms for the oxidative addition of C–Br bonds to Pd(PR3) and Pd(PR3)2 complexes
Paper

Structural isomerism in the [(Ni@Sn9)In(Ni@Sn9)]5− Zintl ion

A new Zintl cluster, [(Ni@Sn9)In(Ni@Sn9)]5−, has been isolated in two distinct isomeric forms, one where both Ni@Sn9 units are coordinated to the bridging indium atom in an η3- mode, the other where one is η3- and the other η4-.

Graphical abstract: Structural isomerism in the [(Ni@Sn9)In(Ni@Sn9)]5− Zintl ion
Paper

Bi- and tridentate stannylphosphines and their coordination to low-valent platinum

Preferential cleavage of Sn–C sp3versus Sn–C sp2 bonds and establishment of trans influence trend SnMe3 > SnPh2(CH2R) > SnPh3 in platinum stannylphosphines.

Graphical abstract: Bi- and tridentate stannylphosphines and their coordination to low-valent platinum
Paper

Tuning the reaction pathways of phenanthroline-Schiff bases: routes to novel phenanthroline ligands

An unusual synthesis of a novel class of tetracyclic diimine ligand and its complexation to rhenium(I) is reported.

Graphical abstract: Tuning the reaction pathways of phenanthroline-Schiff bases: routes to novel phenanthroline ligands
Open Access Paper

Mechanistic insight into novel sulfoxide containing SABRE polarisation transfer catalysts

Mechanistic investigation of sulfoxide based catalysts used to transfer magnetisation from para-hydrogen to pyruvate and oxalate in SABRE.

Graphical abstract: Mechanistic insight into novel sulfoxide containing SABRE polarisation transfer catalysts
Open Access Paper

The role of neutral Rh(PONOP)H, free NMe2H, boronium and ammonium salts in the dehydrocoupling of dimethylamine-borane using the cationic pincer [Rh(PONOP)(η2-H2)]+ catalyst

Cationic σ-dihydrogen, σ-amine-borane and neutral hydride complexes, based upon {Rh(PONOP)}, are all shown play a role in the dehydrocoupling of H3B·NMe2H. Movement between the three is promoted by free amine, NMe2H.

Graphical abstract: The role of neutral Rh(PONOP)H, free NMe2H, boronium and ammonium salts in the dehydrocoupling of dimethylamine-borane using the cationic pincer [Rh(PONOP)(η2-H2)]+ catalyst
From the themed collection: Inorganic Reaction Mechanisms
Paper

Photochemical or electrochemical bond breaking – exploring the chemistry of (μ2-alkyne)Co2(CO)6 complexes using time-resolved infrared spectroscopy, spectro-electrochemical and density functional methods

The photoassisted Pauson–Khand reaction involves the formation of a high-spin diradical species and not CO loss as previously thought.

Graphical abstract: Photochemical or electrochemical bond breaking – exploring the chemistry of (μ2-alkyne)Co2(CO)6 complexes using time-resolved infrared spectroscopy, spectro-electrochemical and density functional methods
Paper

Iridium complexes featuring a tridentate SiPSi ligand: from dimeric to monomeric 14, 16 or 18-electron species

Dimer [Ir{P(o-C6H4CH2SiMe2)2Ph}(μ-Cl)]2 featuring tricoordinate phosphinodisilyl ligands dissociates in solution to the reactive 14 electron monomer [Ir(SiPSi)Cl].

Graphical abstract: Iridium complexes featuring a tridentate SiPSi ligand: from dimeric to monomeric 14, 16 or 18-electron species
Open Access Paper

Transforming PPh3 into bidentate phosphine ligands at Ru–Zn heterobimetallic complexes

P–C/C–H bond activation and P–C/C–C bond formation is observed upon adding ZnMe2 to [Ru(PPh3)3Cl2].

Graphical abstract: Transforming PPh3 into bidentate phosphine ligands at Ru–Zn heterobimetallic complexes
Paper

Controlling the selectivity and efficiency of the hydrogen borrowing reaction by switching between rhodium and iridium catalysts

Fundamental insights into rhodium and iridium catalysed hydrogen borrowing reactions have enabled strategies for controlling product selectivity.

Graphical abstract: Controlling the selectivity and efficiency of the hydrogen borrowing reaction by switching between rhodium and iridium catalysts
Paper

Photolysis of Tp′Rh(CNneopentyl)(PhNCNneopentyl) in the presence of ketones and esters: kinetic and thermodynamic selectivity for activation of different aliphatic C–H bonds

The competitive activation of the various C–H bonds found in ketones and esters by a trispyrazolylborate rhodium complex are compared.

Graphical abstract: Photolysis of Tp′Rh(CNneopentyl)(PhNCNneopentyl) in the presence of ketones and esters: kinetic and thermodynamic selectivity for activation of different aliphatic C–H bonds
27 items

About this collection

This special collection of Dalton Transactions is to mark the 70th birthday of mentor, friend and colleague, Professor Robin Perutz FRS. The collection features areas of organometallic and coordination chemistry where Robin has contributed over the last 40+ years. Themed around the breaking of bonds, it includes both thermal and photochemical bond breakage and activation in stoichiometric and catalytic reactions. Spectroscopic characterisation of reaction intermediates features alongside experimental and computational studies of reactivity.

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