Biosynthesis of the ergot alkaloids
An update on new developments in the field of ergot alkaloid biosynthesis since 2011 is highlighted.
Harnessing non-covalent interactions to exert control over regioselectivity and site-selectivity in catalytic reactions
This perspective examines the progress that has been made in using non-covalent interactions to control regioselectivity and site-selectivity in catalysis.
“Hot or cold”: how do charge transfer states at the donor–acceptor interface of an organic solar cell dissociate?
This perspective discusses concepts to understand efficient photogeneration of charges in organic semiconductors, with particular emphasis on the role of excess energy.
Aerosol-assisted delivery of precursors for
chemical vapour deposition: expanding the scope of CVD for materials fabrication
The aerosol-assisted chemical vapour deposition (AACVD) process is examined, including the influence of deposition conditions on film characteristics and a number of materials and applications to which AACVD has been found beneficial.
Synergistic catalysis: A powerful synthetic strategy for new reaction development
Synergistic catalysis, the simultaneous activation of two reacting partners by discrete catalysts to enable new or elusive chemical transformations, is a valuable synthetic strategy that is growing in popularity. This review seeks to describe the new transformations that highlight the rapid onset of this powerful multi-catalysis concept.
Defect chemistry and electrical properties of sodium bismuth titanate perovskite
We review the diversity of the electrical behaviour of NBT induced by various defect mechanisms, including A-site Na or Bi non-stoichiometry, isovalent-substitution, and acceptor- and donor-doping.
Access to the meta position of arenes through transition metal catalysed C–H bond functionalisation: a focus on metals other than palladium
The elaboration of simple arenes in order to access more complex substitution patterns is a crucial endeavor for synthetic chemists, given the central role that aromatic rings play in all manner of important molecules.
Recent developments of iron pincer complexes for catalytic applications
Iron pincer complexes exhibit excellent activity in homogeneous catalysis.
Aqueous dye-sensitized solar cells
This review highlights the efforts towards the realization of an artificial photosynthetic system able to convert sunlight into electricity by using a unique solvent, water, the solvent of life.
Addition of CF3 across unsaturated moieties: a powerful functionalization tool
This review summarizes recent methodologies for the simultaneous formation of C–CF3 and C–C or C–heteroatom bonds by formal addition reactions to alkenes.
Glycopolymer probes of signal transduction
This review begins with an overview of the structural features of glycopolymers that can affect their recognition by protein receptors and then highlights the use of glycopolymers as probes of signal transduction.
The enzymes of β-lactam biosynthesis
The biosynthetic pathways leading to the different classes of β-lactam antibiotics are reviewed. The mechanisms, structural features and biocatalytic applications of the enzymes involved are highlighted.
Lattice strain causes non-radiative losses in halide perovskites
Halide perovskites are found to exhibit strain patterns over large areas, which influences the lifetimes of charge carriers.
Detection of microRNA biomarkers via inhibition of DNA-mediated liposome fusion
We report the specific and sensitive detection of microRNA using an inverse DNA-mediated liposome fusion assay.
Unlocking the catalytic potential of tris(3,4,5-trifluorophenyl)borane with microwave irradiation
The catalytic activity of tris(3,4,5-trifluorophenyl)borane has been explored in the 1,2-hydroboration reactions of unsaturated substrates.
Photostability of oxazoline RNA-precursors in UV-rich prebiotic environments
Oxazoline precursors of RNA nucleosides are highly photostable molecules and could survive long-term UV-irradiation on the early Earth.
Probing buried recombination pathways in perovskite structures using 3D photoluminescence tomography
Perovskite solar cells and light-emission devices are yet to achieve their full potential owing in part to spatially heterogeneous non-radiative loss pathways that are both on, and buried beneath, the surfaces of films and crystals.
Synthesis and photophysical properties of imine borane adducts towards vapochromic materials
A series of alkynyl aryl conjugated aldehydes and imines were prepared and their adducts with various Lewis acidic boranes have been studied via NMR, absorption, and luminescence spectroscopies in solution.
How to interpret absorption and fluorescence spectra of charge transfer states in an organic solar cell
Energetic disorder is crucial to consistently model both absorption and photoluminescence spectra of charge transfer states in organic solar cells.
Exploring the scope of capacitance-assisted electrochemical carbon dioxide capture
Electrochemical carbon mineralisation is facilitated by the separation of the graphite and aluminium anode components.
Pressure-induced chemistry for the 2D to 3D transformation of zeolites
ADOR, an unconventional synthesis strategy based on a four-step mechanism: assembly, disassembly, organization, and reassembly, has opened new possibilities in zeolite chemistry.
Electrochemical initiation of electron-catalyzed phenanthridine synthesis by trifluoromethylation of isonitriles
Electrochemical initiation of the trifluoromethylation of biaryl isonitriles verifies the electron's catalytic character in the examined cascade reaction.
Reaction monitoring reveals poisoning mechanism of Pd2(dba)3 and guides catalyst selection
We have discovered that the dba ligand in the commonly used Pd2(dba)3·CHCl3 cross-coupling pre-catalyst is susceptible to bis-arylation when used in the presence of aryl iodides.
Bypassing the proline/thiazoline requirement of the macrocyclase PatG
Macrocyclisation of fully non-peptidic compounds and non-heterocycle containing macrocycles using the peptidic ligase PatGmac.
Controlled core-to-core photo-polymerisation – fabrication of an optical fibre-based pH sensor
The fabrication of fluorescence-based pH sensors, embedded into etched pits of an optical fibre via highly controllable and spatially selective photo-polymerisation is described and the sensors validated.
A one-pot tandem chemoselective allylation/cross-coupling via temperature control of a multi-nucleophile/electrophile system
Chemoselective control of a multi-reactive system allows two sequential C–C bond formations via two distinct reactivity modes, accessing pharmaceutical and natural product scaffolds.
Structural characterization of EasH (Aspergillus japonicus) – an oxidase involved in cycloclavine biosynthesis
Aj_EasH is a non-heme iron- and α-keto-glutarate-dependent oxidase that is responsible for an unusual cyclopropyl ring formation in the biosynthesis of the fungal ergot alkaloid cycloclavine.
In situ spectroscopic characterization of a solution-phase X-type ligand exchange at colloidal lead sulphide quantum dot surfaces
We employed quantitative NMR spectroscopy and spectrophotometric absorbance titration to study a quantum dot X-type ligand exchange reaction.
Duplications of an iron–sulphur tripeptide leads to the formation of a protoferredoxin
Based on UV-Vis, NMR, and EPR spectroscopies and DFT and molecular dynamics calculations, a model prebiotic [2Fe–2S] tripeptide was shown to accept and donate electrons.
Cysteine containing dipeptides show a metal specificity that matches the composition of seawater
Cysteine containing dipeptide metal affinities do not follow the Irving–Williams series but rather follow the concentration trends found in seawater.
Enhanced copper-mediated 18F-fluorination of aryl boronic esters provides eight radiotracers for PET applications
Eight clinically relevant radiotracers were isolated applying a Cu-mediated non-carrier added nucleophilic 18F-fluorination of arylboronic ester precursors.
Tunnelling in carbonic acid
The cis,trans-conformer of carbonic acid (H2CO3), generated by near-infrared radiation, undergoes an unreported quantum mechanical tunnelling rotamerization with half-lives in cryogenic matrices of 4–20 h, depending on temperature and host material.
Redox-mediated reactions of vinylferrocene: toward redox auxiliaries
Redox reactions have been used to transform unreactive vinylferrocene into a powerful dienophile and reactive substrate for thiol addition reactions upon conversion to its ferrocenium state.
Tunable and amplified Raman gold nanoprobes for effective tracking (TARGET): in vivo sensing and imaging
We describe the development of a highly tunable, physiologically stable, and ultra-bright Raman probe for in vitro and in vivo surface-enhanced Raman scattering (SERS) applications.
EM∩IM: software for relating ion mobility mass spectrometry and electron microscopy data
EM∩IM enables the calculation of collision cross-sections from electron density maps obtained, for example, by means of transmission electron microscopy. This capability will further aid the integration of ion mobility mass spectrometry with modern structural biology.
Ionic liquids enhance the electrochemical CO2 reduction catalyzed by MoO2
Imidazolium-based ionic liquids promote MoO2-catalyzed electrochemical reduction of CO2.
Band alignment of the hybrid halide perovskites CH3NH3PbCl3, CH3NH3PbBr3 and CH3NH3PbI3
Valence band energies of three organic–inorganic perovskites are compared from electronic structure theory.
Facile synthesis of borofragments and their evaluation in activity-based protein profiling
We describe chemistry that allows synthesis and evaluation of borofragments via conjugation of boron warheads with heterocycles of biological significance.
The identification and characterization of defect states in hybrid organic–inorganic perovskite photovoltaics
Thin film photovoltaic cells based on hybrid halide perovskite absorbers have emerged as promising candidates for next generation photovoltaics.
DNA bioassay-on-chip using SERS detection for dengue diagnosis
A signal-on DNA bioassay-on-chip using SERS detection and a single incubation step without any washing was developed for dengue diagnosis.
Coherent electron spin manipulation in a dilute oriented ensemble of molecular nanomagnets: pulsed EPR on doped single crystals
Pulsed EPR methods are used to carry out nutation experiments on a S = 3/2 molecular nanomagnet doped into a diamagnetic lattice.
Site-selective nitrenoid insertions utilizing postfunctionalized bifunctional rhodium(II) catalysts
Site-selective nitrenoid insertions are made possible with a postfunctionalized dirhodium(II)-catalyst equipped with a remote hydrogen bonding site.
Hybrid mass spectrometry methods reveal lot-to-lot differences and delineate the effects of glycosylation on the tertiary structure of Herceptin®
To quantify the measurable structural heterogeneity of a biopharmaceutical product and the effect of glycosylation on this we systematically evaluate three lots of Herceptin®, two mAb standards and an intact 5 Fc-hinge fragment.
Chiral cyclopentadienyl RhIII-catalyzed enantioselective cyclopropanation of electron-deficient olefins enable rapid access to UPF-648 and oxylipin natural products
Chiral cyclopentadienyl-RhIII complexes catalyze enantioselective cyclopropanations of electron-deficient olefins with N-enoxysuccinimides and are used for syntheses of oxylipins and UPF-648.
Probing surfaces of atmospherically relevant organic particles by easy ambient sonic-spray ionization mass spectrometry (EASI-MS)
EASI-MS is a promising technique for probing the chemical structures of inhomogeneous airborne organic particles.
Mild complexation protocol for chiral CpxRh and Ir complexes suitable for in situ catalysis
Mild complexations of chiral cyclopentadienes with rhodium(I) and iridium(I) precursors enable user-friendly in situ complex formation for catalytic applications.
Phosphorus doped SnO2 thin films for transparent conducting oxide applications: synthesis, optoelectronic properties and computational models
Phosphorus doped tin(IV) oxide (P:SnO2) films, with resistivity values of 7.27 × 10−4 Ω cm and improved visible light transmission, have been synthesised by AACVD.
Diastereoselective C–H carbonylative annulation of aliphatic amines: a rapid route to functionalized γ-lactams
A palladium(II)-catalysed C(sp3)–H carbonylation of free(NH) secondary aliphatic amines to 2-pyrrolidinones is described.
meta-C–H arylation of fluoroarenes via traceless directing group relay strategy
The first example of direct meta-C–H arylation of fluoroarenes to provide valuable meta-fluorobiaryls is achieved by exploiting CO2 as a transient directing group that enables complete regiochemical control of the arylation event.
How can infra-red excitation both accelerate and slow charge transfer in the same molecule?
A UV-IR-Vis 3-pulse study of infra-red induced changes to electron transfer (ET) rates in a donor–bridge–acceptor species finds that charge-separation rates are slowed, while charge-recombination rates are accelerated as a result of IR excitation during the reaction.
A two-qubit molecular architecture for electron-mediated nuclear quantum simulation
A molecular architecture where two vanadyl-based qubits are linked together is herein described and investigated as a platform for quantum simulation.
Chemical structure and bonding in a thorium(III)–aluminum heterobimetallic complex
We describe the syntheses of [Th(III)]–[Al] and [U(III)]–[Al] bimetallics that demonstrate An→Al interactions where the actinide behaves as an electron donor.
Iriomoteolides: novel chemical tools to study actin dynamics
This work broadcasts iriomoteolides as a novel and easily tunable tool for the study of actin polymerization and actin dynamics.
Proteome-wide mapping of PQS-interacting proteins in Pseudomonas aeruginosa
Development and application of chemical probes to globally map key virulence proteins of pathogenic bacteria.
α-Perfluoroalkyl-β-alkynylation of alkenes via radical alkynyl migration
Transition metal-free radical α-perfluoroalkylation with concomitant β-alkynylation of unactivated alkenes is presented.
Solid-state molecular organometallic chemistry. Single-crystal to single-crystal reactivity and catalysis with light hydrocarbon substrates
Solid-state molecular organometallic catalysis (SMOM-cat): synthetic routes, unique structural motifs, mobility in the solid-state and very active gas/solid isomerization catalysts.
Chemoselective oxidation of aryl organoboron systems enabled by boronic acid-selective phase transfer
Chemoselective boronate formation and phase transfer allows chemoselective Brown oxidation of boronic acids in the presence of boronic esters.
The dual role of thiourea in the thiotrifluoromethylation of alkenes
We report the stereoselective and metal-free trifluoromethylation of alkenes followed by S-cyclization using thiourea as the S-source and SET initiator.
The total synthesis of K-252c (staurosporinone) via a sequential C–H functionalisation strategy
A synthesis of the bioactive indolocarbazole alkaloid K-252c (staurosporinone) via a sequential C–H functionalisation strategy is reported.
Extending the biocatalytic scope of regiocomplementary flavin-dependent halogenase enzymes
Targeted mutagenesis increases the activity and alters the regioselectivity of flavin-dependent halogenases.
Studying the active-site loop movement of the São Paolo metallo-β-lactamase-1
A unique structural and biophysical characterization using crystallographic, native ion-mobility mass spectrometry and 19F NMR identifies movement of a loop as being important in SPM-1 catalysis.
oxido incorporation and ligand lability in expanding redox accessibility of structurally related Mn4 clusters
A series of tetramanganese complexes is reported that spans a wide range of oxidation states utilizing a single, flexible ligand architecture.
Development of a generic activation mode: nucleophilic α-substitution of
ketones via oxy-allyl cations
A method for the interception of oxy-allyl cations with a diverse range of common nucleophiles is described thereby demonstrating the value of this intermediate as a generic mode of activation.
Making better decisions during synthetic route design: leveraging prediction to achieve greenness-by-design
A conceptual framework for incorporating machine learned ligand prediction into predictive route comparisons, to enable greener chemistry outcomes.
An efficient synthesis of versatile synthon 3-chlorooxindoles with NaCl/oxone
The present work describes an expedient approach for the direct conversion of indole-3-carboxaldehyde to 3-chlorooxindoles.
Understanding interactions of organic nitrates with the surface and bulk of organic films: implications for particle growth in the atmosphere
Experiments, kinetics modeling and quantum chemical calculations are combined to probe both initial uptake and equilibrium partition coefficients for organic nitrates into various organic films.
Electrical conductivity and conduction mechanisms in (Na0.5Bi0.5TiO3)1−x(BiScO3)x (0.00 ≤ x ≤ 0.25) solid solutions
Large acceptor ions on B-sites are less effective in trapping oxygen vacancies and consequently less effective to suppress the oxide-ion conduction in NBT.
Mobilising ion mobility mass spectrometry for metabolomics
The benefits of adding data from ion mobility measurements to a mass spectrometry based metabolomics workflow are assessed using a panel of small molecules. Data is presented as collision cross section values and distributions.
Bulk synthesis of silver-head colloidal rodlike micromotors
Silver–silica Janus rods synthesized via a pickering emulsion display pronounced self-propelled motion even at ultralow fuel concentrations.
A biocatalytic method for the chemoselective aerobic oxidation of aldehydes to carboxylic acids
Aldehyde dehydrogenases enable the chemospecific oxidation of structurally diverse aldehydes to carboxylic acids in aqueous environment and using only air.
About this collection
In celebration of the 2019 Royal Society of Chemistry prizes and awards, we have collected together some of the exciting research recently published by the winners. This collection showcases articles authored by the winners from across the Royal Society of Chemistry’s journals portfolio – these articles are free to access until 1st August 2019.
Why not also have a look at last year’s collection of articles by our 2018 winners here