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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.
One of the major challenges in C–H functionalization is to achieve selectivity when multiple bonds of similar reactivity are present. Now, a method to selectively amidate sterically and electronically similar β- or γ-C–H bonds that utilize different silver catalysts is reported, giving access to valuable 1,2- and 1,3-aminoalcohols.
Targeted therapy is an important approach to reduce the side effects of medicinal drugs. This work reports the synthesis of catalytically active Pd nanostructures in exosomes that selectively target cancer cells for drug activation using biorthogonal chemistry.
Cu2O is a promising photocatalyst, although its stability is compromised by a disproportionation reaction that leads to the formation of Cu and CuO. Now, a method is reported to stabilize Cu2O nanocubes, rendering them highly active and stable for the photocatalytic reverse water–gas shift reaction.
Elucidating reaction mechanisms on electrode surfaces is of utmost importance. Now, using canonical transition state theory, Cuk and colleagues show the competing pathways by which the charge-trapping intermediates of the water oxidation reaction on n-SrTiO3 decay towards the next step in the reaction.
α-Branched amines are commonplace in pharmaceutical agents. This work reports the synthesis of α-branched amines by simultaneous C–C and C–N bond formation at the sp3 carbon branch site through an 1,1-alkene addition pathway and utilization of three readily accessible starting inputs in a single catalytic cycle.
Traditional modes of catalyst deactivation such as Ostwald ripening and particle migration and coalescence eventually lead to sintering and particle growth. Now, Cargnello and colleagues identify loading-dependent particle decomposition into single atoms as an important deactivation mechanism during methane combustion on colloidal Pd nanocrystals.
Performing photocatalytic CO2 reduction in a selective fashion with molecular catalysts represents a considerable challenge. Here, a binuclear cobalt complex featuring a bi-quaterpyridine ligand is developed that can selectively afford either carbon monoxide or formate by selection of the reaction medium acidity.
C-aryl glycosides are present in many natural products and of interest in drug design, but their chemical synthesis is challenging. This work reports an efficient and diastereoselective ortho-directed C−H glycosylation of arenes and heteroarenes with glycosyl chloride using a palladium catalyst.