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The decoration of surfaces with nanoparticles is typically achieved through deposition, but now John Irvine and co-workers describe a method that gives improved control over particle size, distribution and surface anchorage. They grow nanoparticles at the surface of perovskites through exsolution from the materials' backbones, using variations in non-stoichiometry to tune their properties. The cover shows the scanning electron micrograph of such a surface, in which the metallic nanoparticles have been highlighted with an artificial green colour.Article p916IMAGE: DRAGOS NEAGUCOVER DESIGN: ALEX WING
Processive catalysis is frequent in nature, but much less common in synthetic systems. Now, a semisynthetic biohybrid catalytic system is reported that oxidizes DNA in a processive manner.
Selection of an RNA catalyst that can use the vitamin thiamin to catalyse a key metabolic decarboxylation reaction has broad implications for understanding the role of RNA in the early stages of chemical evolution.
Choosing a solvent for a particular reaction is often a matter of personal preference or the result of limited screening. Now, a computational method allows identification of a solvent that will enhance the kinetics of a reaction prior to running a wet experiment.
The fate of newly created excited states in conjugated materials is not fully understood, with unanswered questions regarding where exactly excitons form and their subsequent behaviour. Now, single-molecule spectroscopy studies of large conjugated molecular wheels reveal that excitons localize at random positions around the wheel rims.
The successes and failures of past research in the development of microfluidic reactors for chemical synthesis are highlighted. Current roadblocks are assessed and a series of challenges for the future of this area are identified.
Surfaces decorated with nanoparticles are typically prepared by depositing particles on the substrate. Instead, particles have now been grown in situ directly from perovskites, by exsolution through judicious tuning of the materials’ compositions, particularly their nonstoichiometry. This approach enables control over particle composition, size, surface coverage and anchorage.
Avoiding the development of microbial antibiotic resistance is a major challenge. Now the incorporation of a photoswitchable group into quinolones has been used to create ‘smart’ antibiotics that can be activated with light. The subsequent loss of activity (within hours) should prevent the build-up of active antibiotics in the environment.
Although much is understood about the mechanical behaviour of macroscopic machinery, less is known about their molecular equivalents. It is now shown that for molecular machinery consisting of hydrogen-bonded components their relative motion is strongly accelerated by adding small amounts of ‘lubricating’ water, whereas other protic liquids have much weaker or opposite effects.
Liquid water has the unique ability to mediate ultrafast energy transfer and relaxation in aqueous chemical reactions. Ultrafast broadband two-dimensional infrared spectroscopy that probes vibrations spanning the mid-infrared region with sub-70-femtosecond time resolution now provides evidence for highly intertwined intra- and intermolecular vibrations in water that act to efficiently dissipate vibrational energy.
Positron emission tomography imaging is an increasingly important technology in drug discovery and development, so there is an urgent need for logistically simple processes that allow access to [18F]CF3 (hetero)arenes. Here, a late-stage [18F]trifluoromethylation of (hetero)aryl iodides from [18F]fluoride and commercially available reagents is described, a process that relies on the in situ preparation of [18F]CuCF3.
Clamp proteins that encircle DNA and then recruit enzymes are one of nature's ways of making catalysis on DNA processive. Here, a clamp protein is equipped with a synthetic catalyst that sequence-specifically oxidizes DNA. The resulting biohybrid catalyst shows processive behaviour, which is visualized by atomic force microscopy.
Finding the right solvent can radically transform the rate of a reaction. Here, a systematic computational method for the identification of solvents that accelerate kinetics is described. Starting with a quantum mechanical computation of the reaction rate constant in a set of six solvents, a computer-aided approach identifies the best solvent among 1,341, with a 40% increase in reaction rate.
Immobilized microfluidic water-in-oil droplets serve as templates for layer-by-layer deposition of lipid monolayers to create vesicles of programmable lamellarity and content. Arrays of vesicles allow reproducible assembly and multi-vesicle probing of complex membrane-associated parameters, such as permeability, asymmetry and membrane protein function.
A deficiency in our molecular-level understanding of the electronic structure of conjugated polymers hinders their potential use in electronic applications. Shape-persistent highly ordered ring structures have been used to mimic conjugated polymers and have now been studied using single-molecule spectroscopy. The fundamentally non-deterministic nature of excitation energy localisation in π-conjugated macromolecules has been demonstrated.
Vitamins are thought to be relics of a primordial RNA World. A demonstration that catalytic RNAs are capable of harnessing vitamin cofactors would support the likely role of vitamins in early metabolic processes. Here, a ribozyme that uses vitamin B1 to aid decarboxylation of a pyruvate-like substrate is reported.