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The synthesis of tri- and tetra-aryl alkenes is limited by poor regio- and stereoselectivity. Here MIDA boronate-substituted aryl alkynes are used to achieve regioselective three-component diarylation of the alkyne and to provide a cross-coupling handle for subsequent elaboration to tri- or tetra-substituted products.
There is a continuous demand to develop new procedures for the synthesis of pristine graphene for device applications. Here the authors report gold catalyzed in situ formation of graphene from hydrocarbon contaminants in a transmission electron microscope within a few milliseconds at room temperature.
Despite extensive investigation, the force-dependent unfolding/rupturing rate of biomolecules still remains poorly understood. Here the authors apply Kramers kinetic rate theory to a model system showing that catch-to-slip switch behaviour can be understood in a one-dimensional energy landscape.
Nickel-catalysed C-H functionalisation reactions are of increasing importance. Here the mechanism of Ni(II)-catalysed C-H arylation of amides is shown to depend on the nature of the oxidant and in particular the energy of its Caryl-I antibonding orbital.
The direct glycosylation of ribose by nucleobases offers an intuitive route to nucleosides, but is known to be challenging under prebiotically plausible reaction conditions. Here, the addition of amino acids is shown to influence the product distribution, and a dynamic exchange of nucleobases between nucleosides and nucleotides is observed.
It is important to identify heterogeneous catalyst compositions which minimize use of precious metals. Here the authors analyse the size-activity behaviour of platinum-based formaldehyde oxidation catalysts, identifying a volcano relationship with nanometer scale nanoclusters being the most effective.
Mechanically interlocked molecules are widely studied, but the pathways by which they assemble are less well understood. Here the formation process of a quadruply-locked Pd4L8 cage is studied by NMR and mass spectrometry, with intermediates inferred by kinetic analysis.
Fluorinated solvents such as hexafluoroisopropanol (HFIP) are often useful in reactions involving radical cations. Here the role of HFIP in photoredox and electrochemical Diels-Alder reactions is explored experimentally and theoretically, and attributed to solvation of anions to reduce their nucleophilicity.
The Strecker reaction is thought to offer a prebiotically plausible synthesis of amino acids, but is reversible at the high or low pH ranges needed to promote reactivity. Here the reaction of hydrogen cyanide and diamidophosphate is shown to provide stable phosphorylated amino acid precursors at neutral pH, which can be hydrolysed to amino acids or thiolysed to thioamides.
Probing intermolecular interactions and film heterogeneity in organic semiconductors is challenging. Here, the authors use micro-Raman spectroscopy to assign vibrational modes of isomerically pure functionalized anthradithiophenes, which are then used to image crystalline sub-domains in mixed-isomer samples.
Isoprene is a key compound emitted into the atmosphere, which reacts rapidly with hydroxyl radicals and contributes to aerosol formation. Here the authors conduct flow tube measurements to observe the early stages of isoprene oxidation product formation in low hydroperoxy radical and nitric oxide environments.
Structural phase transitions induced by external stimuli play crucial roles in controlling the functions of solid-state materials. Here the authors report the photo-triggered phase transition of a photochromic chiral salicylideneamine crystal, and probe the local effects driving the transition.
The ceramide transport protein CERT is of potential therapeutic interest but is typically targeted using ceramide-derived ligands. Here the authors use virtual screening and a quantitative surface plasmon resonance assay to identify ceramide-nonmimetic inhibitors of a CERT subdomain and test their activity in live cells.
Stable single-atomic and noble-metal free catalysts are crucial in light driven hydrogen evolution but their behavior upon visible light irradiation remains unclear. Here the authors develop and analyze atomic palladium on graphitic carbon nitride with enhanced catalytic activity under visible light.
The oxidative cleavage of the C–C bonds in 1,2-diols is an important transformation but lacks a recyclable, mild aerobic catalytic system. Here the authors present atomically dispersed cobalt on N-doped carbon to deliver improved catalytic activity and recyclability, and probe the reaction pathway.
Several catalytic methods for N-formylation of amines using noble metals or manganese pincer complexes are known. Here an air-stable and reusable chromium-based polyoxometalate is shown to catalyze the N-formylation of amines and diamines using methanol and hydrogen peroxide.
Copper(II)-superoxide complexes are known to behave as electrophiles but there are few examples of nucleophilic reactivity by such species. Here a mononuclear copper(II)-superoxide species is shown to promote simple aldol reactions, and this reactivity is found to be sensitive to minor changes to the ligand structure.
Phase change random access memory relies on phase transformation, from a metastable rock salt structure to a stable hexagonal structure, details of which remain unclear. Here the authors use atomic resolution energy dispersive X-ray spectroscopy to probe the atomic-level rearrangements during the phase transition.
Oxygen vacancies in metal oxide based catalytic materials are pivotal to improving their performance. Here the authors use density functional theory and experimental data to show that introduction of hydroxyl groups in clay-supported cobalt oxides can introduce oxygen vacancies and enhance its catalytic activity.