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The asymmetric hydrogenation of alkenes is a common route to optically active compounds, but alkene synthesis is often atom-inefficient, and the formation of isomers further complicates the procedure. Now the Ir-catalysed deoxygenation of racemic alcohols is shown to be a simple route to enantioenriched products.
Photocatalytic activation of alkyl carbon–chlorine bonds has constantly proven difficult due to the high energies needed to cleave this stable bond. Here a surfactant-based photocatalytic system is used, allowing for the radical dehalogenation and subsequent reactivity of unactivated alkyl chlorides.
Deuterated molecules are important both as labelled probes and as targets in their own right. Here the authors report a very simple and general deuteration of aldehydes, by the use of an N-heterocyclic carbene catalyst in the presence of D2O.
Due to its stability nitrogen is often employed as an inert gas during catalytic reactions. Now, a study shows that N2 can act as promoter for the catalytic hydrodeoxygenation of p-cresol on supported ruthenium catalysts through the formation of hydrogenated nitrogen species acting as a source of protic hydrogen.
This work shows that the biosynthesis of the polyether tetronasin involves an apparent enzyme-catalysed inverse-electron-demand hetero-Diels–Alder reaction to form an unexpected oxadecalin intermediate. A second enzyme then rearranges the oxadecalin to form the four-ringed tetronasin.
To achieve large-scale application of water electrolysers we need to find optimal cathode and anode catalysts. This work reports an engineered silver catalyst with high density of stacking faults that exhibits high activity and stability for the hydrogen evolution reaction, outperforming commercial platinum on carbon.
Visualizing catalysts at work poses significant experimental challenges. Here, an operando scanning tunnelling microscopy study of the cobalt-catalysed Fischer–Tropsch synthesis is presented, which establishes steps as the active sites of the process by correlating activity under realistic conditions with step density.
Selective functionalization of C(sp3)–H bonds is difficult in alkanes and other hydrocarbons, and especially so for enantioselective reactions. Here the authors report a photocatalyst and chiral metal catalyst to allow the radical, asymmetric addition of alkyl, allylic and benzylic groups to imines.
Reductive desymmetrization of 2,2-disubstituted cyclodiketones can provide valuable complex molecules with multiple chiral centres, but the generation of a single stereoisomer is difficult. This work addresses this synthetic challenge by engineering the activity and stereoselectivity of a carbonyl reductase.
Lithium-ion batteries exhibit high theoretical gravimetric energy density but present a series of challenges due to the open cell architecture. Now, Zhou and co-workers confine the reversible Li2O/Li2O2 interconversion into a sealed cell by pre-embedding Li2O nanoparticles into an iridium–graphene catalytic host.
Tackling the loss of expensive cofactors is a key challenge in continuous-flow biocatalysis. This work reports immobilized enzymes with a tethered cofactor that is channelled between a recycling and a catalysis module facilitating total turnover numbers of NAD+ and ATP exceeding 10,000 in biocatalytic flow systems.
Asymmetric routes for the formation of tetrasubstituted allenes are scarce and limited in scope. Now, a catalytic asymmetric process is reported giving access to tetrasubstituted allenes from readily available propargylic alcohols, and a potential role for an achiral supporting ligand is postulated.
Enantioselective synthesis of atropisomeric biaryls is highly desirable due to the utility of these compounds as ligands and catalysts. Now, an organocatalytic polyketide cyclization is shown to convert poly-β-carbonyl compounds into binaphthalene derivatives in good enantioselectivities.
Multi-modal approaches to simultaneously characterize different aspects of a reaction in situ are not readily accessible. Here, catalyst extrudates equipped with both luminescence thermometry and Raman spectroscopy sensors are introduced, providing an in-depth picture for the conversion of syngas on a supported rhodium catalyst.
Due to its importance, the water-gas shift reaction has been the subject of numerous studies; however, a unifying mechanistic picture has not yet emerged. Now, a combination of spectroscopic, kinetic and computational methods reveal the crucial role of carboxyl intermediate for this centuries-old process.
Simple enzyme mimetics are highly desired for industrial settings providing high catalyst stability and low production costs. This work reports that phenylalanine and zinc ions can self-assemble into a supramolecular structure showing catalytic properties similar to those of the natural enzyme carbonic anhydrase.
Imine reductases have been regarded as one of the most promising enzymes by the pharmaceutical industry—but their industrial application is still lacking. This work reports the successful industrial application of an imine reductase, enabled by directed evolution.
Small changes in catalyst synthesis can have large and often poorly understood effects on activity. Here the authors show how variation of post synthetic heat treatment—in combination with changes in metal loadings—can lead to the most efficient catalysts, and also identify the most likely active sites.
Directed evolution typically requires extensive screening. This work presents an ultrahigh-throughput microfluidic assay, based on a coupled reaction and fluorescence-activated droplet sorting, enabling a 960-fold activity improvement of an amine oxidase for a non-natural substrate in a single round.
Here the enantioselective lithiation of Boc-1,3-oxazinanes is reported. Transmetallation to zinc allows for regiodivergent functionalization at either C4 or C5 positions via a ligand-controlled Negishi coupling, and subsequent oxidative cleavage gives easy access to both β2- and β3-amino acids.