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Partially oxidised pillar[n]arenes exhibit interesting redox behaviour, but the pillar[6]arenes are poorly characterised in this context. Here stepwise oxidation of 1,4-diethoxypillar[6]arene allows detailed study of the structural and electrochemical properties of molecules with 2, 3, and 4 oxidised units.
A comprehensive understanding of soot nucleation in flame combustion is still lacking. Here the authors identify homo- and heterodimers of small-to-moderate size polycyclic aromatic hydrocarbons in the gas to soot transition region of a laminar diffusion methane flame as viable intermediates in the soot nucleation process.
Nucleic acid probes that bind to cancer-related genes have potential as diagnostic tools. Here parameters governing the binding of locked nucleic acid probes to three oncogenes, including effects of molecular crowding and polyelectrolytes, are characterized and used to inform the design of a bead-bait RNA genotyping assay.
Lipoarabinomannan is a carbohydrate expressed on mycobacterial cell surfaces and implicated in host-pathogen interactions, but its structure is not well-characterised. Here mass spectrometry studies of enzymatic digests reveal the presence of secondary extended mannan pendants and indicate a revised structure for the connectivity of the core domains.
Multidimensional NMR spectroscopy can provide insight into the unfolding of proteins in cells, but may be sensitive to the choice of residue used as a reference. Here 2D 1H-15N NMR is used to obtain thermodynamic parameters of unfolding of Yfh1, relying on an internal standard to normalise peak volumes.
The radical C–F cleavage of fluoroalkanes offers a valuable method for the synthesis of fluorinated products. Here, photoredox catalysis promotes tandem intermolecular defluoroalkylation/intramolecular heteroaryl migration of unactivated alkenes to yield difluorobenzyl ketones, proposed to proceed via a radical mechanism.
Intramolecular ring-opening metathesis oligomerisation is a useful method for constructing multicyclic polymer cages. Here, it is applied to the synthesis of spirocyclic polymers with figure-8, trefoil, and quatrefoil structures with low polydispersity.
Soft x-ray magnetic circular dichroism is typically used to study ferro- or paramagnetic materials, but not diamagnetism. Here XMCD fine structures are used to distinguish diamagnetic states in molecular polyoxopalladates in conjunction with theoretical calculations.
The reaction of HO2 radicals with NO is a critical part of the atmospheric ozone cycle, but the plethora of involved species makes it hard to fully decipher. Here, quantitative and simultaneous determination of multiple reaction species, including HO2 and OH radicals, is achieved by means of high-resolution time-resolved dual-comb spectroscopy.
Bicyclic aromatic olefins are promising chromic materials but the equilibrium between their folded and twisted conformers is not well understood. Here, a combination of experimental and computational methods allows measurement of the equilibrium constants and thermodynamic parameters, offering insight into their chromic behaviour.
The modular synthesis of crowded alkenes is a challenge. Here diaryliodonium salts are used to arylate vinyl boronates, which can then undergo Suzuki-Miyaura coupling with the aryl iodide generated in situ in the first step to yield modular trisubstituted alkenes.
Organophosphorous zwitterions are important intermediates in organic synthesis but can be unstable and difficult to characterise. Here, two analogues of such intermediates stabilised by conjugation to an open-cage fullerene derivative allow for characterisation by single-crystal X-ray diffraction, with mechanistic implications.
Sequestration of CO2 in geological reservoirs holds great potential, but ex situ mineral carbonation generally requires harsh, energy-intense conditions. Here the authors study CO2 physisorption at open nanospaces within overlapping nanosheets in saponite clay under ambient conditions.
Water ligands found in the oxygen-evolving Mn4CaO5 cluster in photosystem II are thought to be important during photosynthesis, but the nature of the proton-releasing substrate water molecules is disputed. Here the pKa values of four key water molecules are estimated, with implications for the mechanism of water oxidation.
Acomplete account of the structural evolution occurring during photopolymerisation is lacking. Here the physical changes occurring on the nanometer scale during photopolymerisation of acrylates are followed over time by FTIR, X-ray reflectometry, AFM, and GISAXS, offering insight into the mechanism by which initial composition influences the final morphology.
For the geological disposal of radionuclides through immobilization within minerals, naturally aerobic conditions need to be considered. Here the authors report a quantitative reduction of Tc7+ and partial structural incorporation of Tc4+ into in situ formed nonstochiometric magnetite under ambient conditions.
Microwave irradiation allows for direct and focused heating of solid catalysts, however, temperature control remains a major challenge. Here the local temperatures of platinum nanoparticles on γ-Al2O3 and SiO2 supports are elucidated with in situ XAFS and operando XANES spectroscopy.
Nurr1 is a promising therapeutic target for neurodegenerative diseases, but mechanistic understand of its modulation is limited and Nurr1 modulators as tools are lacking. Here, non-steroidal anti-inflammatory drugs are shown to act as inverse Nurr1 agonists, and their interactions with the NR4A family are characterised.
The properties of carboxyl compounds depend on their conformations, but characterising each conformation can be challenging. Here, femtosecond spectroscopy reveals that the carboxyl group of N-acetylproline preferentially adopts a syn conformation in water, but in apolar environments an intramolecular hydrogen favours an anti conformation.
Degradation of heterogeneous catalysts limits their cost efficiency and sustainability. Here a hydrogenation catalyst that is stable over a hundred cycles of reuse is reported, with stability attributed to the formation of an agglomeration at the palladium/silicon interface.