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The use of electrochemistry in asymmetric catalysis can prove challenging, not least due to the difficulty of achieving chemo- and stereoselectivity in combination with very reactive electrochemically generated intermediates. Here, catalytic asymmetric electrosynthesis is reported for the synthesis of 1,4-dicarbonyl compounds with high enantiomeric excess, including compounds with all-carbon quaternary stereocentres. The chiral-at-metal catalyst activates the substrate towards anodic oxidation in addition to controlling the enantioselectivity of the process.
Reusable catalysts based on earth-abundant metals could offer inexpensive and sustainable routes in organic synthesis. Here a nickel catalyst—formed by pyrolysis of a nickel complex on a γ-Al2O3 support—is shown to be highly active for synthesis of primary amines via reductive amination. The catalyst operates with aqueous ammonia and either aldehydes or ketones, tolerating a wide range of functional groups.
The electroreduction of carbon dioxide to formate represents a
desirable strategy for the production of fuels and commodity chemicals. Now, guided
by density functional theory, Cui and colleagues report CuSn3
alloys that exhibit high activity and selectivity for formate production from
CO2 electroreduction at potentials as low as −0.5 V versus
RHE.
Copper-based catalysts, especially the so-called oxide-derived copper, are capable of producing multicarbon species from electrochemical CO2 reduction. However, little is known about their active sites despite intensive research efforts. Now, Lum and Ager show that oxide-derived copper catalysts have three distinct product-specific sites for the formation of C2+ chemicals, unlike polycrystalline copper or (111)- and (100)-oriented copper films which show no evidence of product specific sites.
Nanoscale texture of electrocatalysts, enabled by the tools of nanoscience, is emerging as an important lever for the control of electrochemical reaction pathways.
A crucial malonic acid moiety in the antibiotic malonomycin has been shown to be installed by a bacterial vitamin K-dependent (VKD) carboxylase orthologue.
The biosynthesis of the pharmacophoric tetrahydropyran of the clinically important antibiotic mupirocin remained enigmatic for a long time. Now, research shows that this ring is formed by a unique epoxidation–epoxide-opening cascade starting from a non-activated alkane.
Single-atom catalysts recently attracted considerable research interest for heterogeneous electrocatalysis, including the oxygen reduction reaction. Now, an intriguing two-step approach towards a less explored atomic nitrogen-coordinated manganese with a high loading density has been developed.
Single-atom catalysts are very attractive due to their ability to maintain high activities at the lowest possible precious metal loading. Here, a double transition metal MXene that effectively anchors single Pt atoms is reported, and exhibits superior performance and stability towards the hydrogen evolution reaction.
Predicting highly enantioselective ligands for a given asymmetric catalytic reaction is very challenging, but could greatly reduce the need for high-throughput, trial-and-error experimentation. Here, the authors report a freely available, automated tool to identify appropriate chiral ligands for given substrates in asymmetric catalysis.
Unlike the more common C–H functionalization, methods for the functionalization of C–C bonds are scarce. Here, Ackermann and co-workers show that an inexpensive manganese catalyst is capable of selectively activating C–C bonds for alkylations, alkenylations, and allylations in water.
Catalysts are dynamic species, whose structure can change over the course of a reaction. Here, structural changes are mapped for cobalt–palladium nanoparticles during CO oxidation, showing a reconstruction to CoOx on palladium surfaces. Furthermore, the composition-dependent reconstruction can be correlated with the trend in catalytic activity.
One of the major routes for the use of CO2 in chemical production is the formation of carbonates via cycloaddition of CO2 to epoxides. This work uses a range of experimental and computational techniques to map out the elusive key intermediates in this process.
The electrochemical reduction of carbon dioxide allows recycling of the greenhouse gas to produce chemicals and fuels. In this Review, Seh and co-workers discuss the progress in operando techniques applied to heterogeneous carbon dioxide electroreduction, highlighting the mechanistic insights that these techniques have provided.
Two-dimensional materials have been in the spotlight since the discovery of graphene, and over time an extensive library of other ultrathin layered structures have emerged. In this Review, Pumera and Chia gather and discuss the features of this class of materials and review their recent applications in electrocatalysis.
Mupirocin is a clinically important antibiotic, but the biosynthesis of its tetrahydropyran moiety—an oxygen heterocycle essential for its bioactivity—has remained elusive. Here, Willis, Crump and co-workers report an enzymatic reaction cascade catalysing this ring formation from a non-activated C–H bond.