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One-pot processes in which a single catalyst carries out several reactions are attractive, but typically promote the formation of by-products as well as the desired ones, and are not amenable to optimization of the individual transformations. Now, these issues have been overcome by separating the catalytic processes in time.
Fluorine imparts many drugs with beneficial properties, however, the synthesis of fluorinated complex natural products is challenging. Biosynthetic strategies and recent experimental precedents have paved the way for bioengineered fluorinated polyketides.
Quantitatively studying how the rate of a chemical reaction is affected by a reactant's atomic-scale environment is extremely challenging. This has now been achieved at the single-molecule level using scanning tunnelling microscopy to monitor tautomerization in an atomically well-defined environment.
Replication of the HIV-1 viral genome can be inhibited by a protein known as APOBEC3G, via two seemingly contradictory mechanisms. Now, the molecular conundrum behind these two processes has been resolved.
Lengthy molecular dynamics simulations of complex systems at the atomic scale usually require supercomputers. Now, by stitching together many shorter independent simulations run 'in the cloud', this requirement has been circumvented, allowing two milliseconds of the dynamics of a G-protein-coupled receptor to be simulated.
Using chemical reactions and diffusion to control pattern formation requires the careful design of reaction networks and a balance of kinetics that is difficult to achieve. Now, it has been shown that DNA-based reaction networks provide a robust method for transforming patterns.
An RNA replicase ribozyme has long been sought by chemists interested in the origin of life. Now, a selection strategy employing a low-temperature water–ice mixture as the medium has led to discovery of a ribozyme that can catalyse polymerization of an RNA chain greater than its own length.
Mastering how to completely control the exact monomer sequence of synthetic polymers is the ultimate key for establishing true biomimetic macromolecular chemistry. A versatile one-pot approach for the synthesis of well-defined multiblock copolymers with short block lengths offers another approach on the road towards this lofty goal.
London dispersion forces have been cited as an important factor in protein folding, drug–receptor interactions, and catalyst selectivities. However, careful analysis of a model system finds that the dispersion interactions are only minor contributors to the formation of complexes in solution.
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.
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.
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.
Millimetre-sized single crystals of covalent organic frameworks have been constructed by taking advantage of a reversible dimerization reaction of nitroso groups.
Although caesium is well known in its oxidation state +I, many chemists have speculated about a possible higher state. Such a species has not yet been prepared, but based on quantum-chemical calculations CsFn compounds have now been predicted to be stable.
Preparing powerful reactive intermediates such as enolates and homoenolates for C–C bond formation used to require strong bases and stoichiometric reagents. They can now be catalytically generated from α-functionalized aldehydes or even from saturated esters under mild conditions using N-heterocyclic carbene catalysts.
Covalently bonding groups to the walls of carbon nanotubes has been previously observed to quench their photoluminescence. Now, it has been shown that, if you get the chemistry just right, their photoluminescence can in fact be significantly brightened by introducing defects through functionalization.
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.
A nanographene compound incorporating five- and seven-membered rings is found to have a highly distorted non-planar structure and serves as a model system for studying the effect of defects in graphene sheets.
Chemical reactions with activation barriers generally slow to a halt in the extreme cold of dense interstellar clouds. Low-temperature experiments on the reaction of OH with methanol have now shown that below 200 K there is a major acceleration in the rate that can only be explained by enhanced quantum mechanical tunnelling through the barrier.
