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Transition metal-catalysed bioorthogonal reactions are severely hindered in biomedical applications, mainly due to a lack of target specificity. Now, research shows that a trojan exosome vesicle can deliver a palladium catalyst specifically to progenitor cells for bioorthogonal catalysis, allowing localized prodrug activation.
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.
While the oxidative addition of Pd to carbon–halide bonds is often regarded as being essentially irreversible, this is sometimes not the case. This Perspective looks at the conditions leading to reductive elimination of Pd from carbon–halide bonds, and the synthetic opportunities that this offers are discussed.
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.
Fusion systems have been designed that link enzymes to cofactors and immobilization modules through appropriate synthetic spacers. These modular biocatalysts (assembling catalysis, cofactor provision/regeneration and assisted immobilization) are suited to heterogeneous biocatalysis systems and can be efficiently used in continuous flow reactors.
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.
Conventional experiments for generating proteins with improved properties by directed evolution are iterative, lengthy and costly. Now, a label-free assay has been developed for ultrahigh-throughput microfluidic screening that can dramatically accelerate the discovery of superior biocatalysts from a single round of genetic randomization.