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Efficient autoxidation of organic compounds typically requires that they possess double bonds or oxygen-containing moieties, which is why alkanes were thought to contribute little to atmospheric organic aerosol formation. Here, mass spectrometry shows significant autoxidation of alkanes under both atmospheric and combustion conditions.
Portable liquid chromatography instruments enable a myriad of applications in field research. Here a handportable system incorporating a broadband absorption detector is used to separate and classify polycyclic aromatic hydrocarbons from environmental water samples based solely on spectral fingerprinting.
Recent works have highlighted the role of energy sources in driving nonequilibrium behaviours in chemical reaction networks. Here, the authors theoretically describe linear reaction networks with thermal gradients to highlight the basic rules governing most favourable states, relating them to kinetic and dissipation rates.
Despite strong demand for their clinical use, the synthesis of heparin oligosaccharides as anticoagulants remains challenging. Here, a mild and scalable formal synthesis of Fondaparinux pentasaccharide is presented through [Au]/[Ag]-catalyzed glycosidations.
Collision geometries are hard to control, making transition states in chemical reaction hard to study. Here the authors show that a linear transition state leads to formation of reaction product ‘knocked-on’ along the continuation of the direction of reagent approach.
Cyanide anions exist in interstellar space, but the vibrationally or electronically excited states above the electron autodetachment threshold of CN- are assumed to have no contributions to cosmic CN-. Here, the authors report long-lived, superexcited CN- from the dissociative electron attachment to cyanogen bromide.
Methacrolein oxide is one of the ozonolysis products of isoprene present in our atmosphere, but its relevance under humid conditions is not fully understood. Here, UV-vis spectroscopy and reaction kinetics studies show much longer lifetimes of anti-methacrolein oxide than previously thought, suggesting much higher steady-state concentrations and higher impact on the oxidation of atmospheric SO2.
The chemical space of prebiotic chemistry is extremely large, while extant biochemistry uses only a few thousand interconnected molecules. Here we discuss how the connection between these two regimes can be investigated, and explore major outstanding questions in the origin of life.
Nano-sized catalysts are useful for electrocatalytic nitrogen reduction, but loading the particles on electrode substrates can limit catalytic performance. Here, the authors report nitrogen to ammonia electroreduction mediated by silver nanodots dispersed in an aqueous solution.
Molten salt electrolytes are widely used in energy storage and conversion, but our understanding of conductivity trends remains incomplete. Here, computational approaches are used to determine ionic electrical mobilities, local structures, and kinetics, unravelling the origins of conductivity in molten lithium halide salts.
Methyl vinyl ketone oxide is an important Criegee intermediate formed during the ozonolysis of isoprene, but its formation and resonance stabilization remain poorly characterized. Here, transient infrared spectroscopy of the syn-trans-conformer shows a stronger O‒O stretching band at 948 cm-1 that confirms the stabilization.
Under-coordinated corner and edge sites often dictate oxide properties, however, information about their atomic-scale structure and chemical nature is often missing. Here, a combined experimental and theoretical study of the ZnO(10-14) surface reveals stable, long-range ordered, non-polar facets of ZnO, with a high step-density and uniform termination.
Natural gas can be collected from hydrate deposits by exchange with CO2, but the ensuing mixed hydrates and the path to a complete exchange are not fully understood. Here, computational analyses of neutron pair distribution functions of CH4, CO2 and mixed CH4-CO2 hydrates at 10 K reveal that the behavior of mixed gas species cannot be interpolated from properties of pure compounds.
Rutile TiO2 is a prominent photocatalyst for overall water splitting, but the on-surface activation of hydrogen atoms is still not fully understood. Here, the authors use atomic force and kelvin probe force microscopy to study the lateral manipulation of hydrogen on a rutile (110) surface.
Octacalcium phosphate is a precursor to a key component of human bone and tooth enamel which can incorporate carboxylate species, but the effect of multivalent carboxylates is not well understood. Here the incorporation of tetracarboxylic acids into OCP is shown to influence the structural and optical properties of the resultant composite.
Biomineralization allows for crystal structure, size, and morphology control over inorganic compounds, but precipitation at random compositions hinders the construction of complex nanostructures. Here, the elemental composition of a gold-titania nanocomposite photocatalyst is controlled through two inorganic precipitating peptides bound to DNA.
Metal–organic frameworks have been shown to adsorb and decompose chemical warfare agents, but their mechanism of action is not completely understood. Here the authors quantitatively track the binding and decomposition product structures of nerve-agent simulant dimethyl methylphosphonate in host UiO-67 through in situ X-ray total scattering measurements, pair distribution function analysis, and density functional theory calculations.
Near-infrared fluorescent proteins engineered from bacterial phytochromes are important for deep-tissue imaging in vivo, but the mechanism through which they bind to chromophores is not fully understood. Here the authors structurally analyze biliverdin binding to miRFP proteins using time-resolved stimulated Raman spectroscopy and quantum mechanical/molecular mechanics calculations.