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Forming carbon–carbon bonds at the expense of two C–H bonds is difficult, but attractive, as it reduces the number of chemical steps during synthesis by avoiding prefunctionalization. Here such a method is reported, involving an interrupted Pummerer reaction and a photoredox-catalysed coupling.
Efficient microbial production of medium-chain fatty acids (MCFAs; C6–C12)—valuable molecules in the oleochemical and biofuel industry—is challenging due to their cellular toxicity. Now, this work improves the production of extracellular MCFAs to over 1 g l−1 by systematically engineering yeast at multiple levels.
Dry reforming of methane can so far afford syngas with equimolar CO and H2, which is suboptimal for Fischer–Tropsch chemistry. Now a process is reported based on a Ni–In molten metal alloy catalyst that is capable of producing syngas with practically relevant H2/CO ratios together with separable carbon.
The organocatalysed addition of aldehydes to nitroolefins is an extremely well-studied reaction that almost exclusively provides the syn-configured products. Here a general method to reverse the diastereoselectivity is reported, whereby a tripeptide catalyst consistently provides the anti product with high selectivity.
Amide reduction via hydroboration is challenging, and catalysts often exhibit limited substrate scope. Here the authors report synthesis of a lanthanum cluster as a catalyst for the hydroboration of esters and amides, capable of reducing a wide range of primary, secondary and tertiary amides to amines.
In order to use early, non-noble transition metals in homogeneous catalysis, complex ligands are typically needed, offsetting the benefits of inexpensive metals. Here the authors show that a simple manganese complex can be used in the hydrogenation of N-heteroarenes, without the need for additional ligands.
Electrochemical 2e− water oxidation is a promising route for renewable H2O2 production but it suffers from low selectivity due to the competing 4e− process. Here the authors demonstrate an interfacial engineering approach where the catalyst is coated with a hydrophobic polymer to confine in situ produced O2 and promote the 2e− pathway.
Investigation of proximity-driven enzyme regulation in intracellular signalling could benefit from suitable model systems. This work reports the engineering of a synthetic DNA origami-based apoptosome facilitating detailed analysis of caspase-9 activation, which is essential in programmed cell death.
Ethylene glycol is a commodity chemical with an annual consumption of 20 million tonnes. Its production generates 1.6 tonnes of CO2 per tonne of ethylene glycol. To reduce these CO2 emissions, the authors report a one-step electrochemical route to selectively convert ethylene to ethylene glycol at ambient temperature and pressure in aqueous media.
Identifying rate-determining steps (RDSs) is one of the most challenging aspects of catalysis. This work presents a general framework to identify the RDS of mixed ion and electron transfer reactions, and applies it to the four-electron/two-ion O2 reduction in solid-oxide fuel cell cathodes, converging on four RDS out of more than 100 possible candidates.
Late-stage aromatic chlorination of active pharmaceutical ingredients has enormous potential in drug discovery yet still features limited applicability due to issues of functional-group tolerance. Now, dimethyl sulfoxide is reported as catalyst for the chlorination of a diverse family of bioactive molecules in combination with N-chlorosuccinimide.
The rational design of catalysts is crucial to make power-to-X technologies viable. Here the authors introduce the delafossite PdCoO2 as a highly active hydrogen evolution reaction catalyst due to the growth of a tensile-strained Pd-rich capping layer under reductive conditions. Image credit: Christop Hohmann.
Electrocatalytic reduction of CO2 to multicarbon products is useful for producing high-value chemicals and fuels. Here the authors present a strategy that is based on the in situ electrodeposition of copper under CO2 reduction conditions that preferentially expose and maintain Cu(100) facets, which favour the formation of C2+ products.
In situ studies of catalytic surface reactions are restricted to a small number of analytical techniques. Here, scanning electron microscopy is utilized to visualize the catalytic hydrogenation of nitrogen dioxide on platinum, showing its potential for monitoring reaction dynamics on surfaces.
Electrochemical conversion of CO2 into liquid fuels, powered by renewable electricity, offers one means to address the need for the storage of intermittent renewable energy. Now, Sargent and co-workers present a cooperative catalyst design of molecule–metal interfaces to improve the electrosynthesis of ethanol from CO2 by producing a reaction-intermediate-rich local environment.
Enzyme engineering is opening up new chemistries. Here, the authors report enzymes engineered to contain two biological active sites — also showing that one site can be converted to a metal-complex catalyst — and demonstrate the utility of such dual sites in a range of catalytic processes.
Nickel complexes are of ever-increasing importance in organic synthesis; however, unstable Ni(COD)2 is still the main Ni(0) source used. Here the authors report a solution to this long-standing issue: an air stable Ni(0) complex that acts as a general precatalyst for numerous nickel-catalysed reactions.
Additions to alkenes and alkynes are useful routes for generating highly functionalized products. Here the authors report the 1,1-difunctionalization of alkynes through a CuH-catalysed asymmetric hydroboration/hydroamination cascade.
Methods to allow access to all isomers of a product are both valuable and challenging to achieve. Here the authors report a catalytic system comprised of an N-heterocyclic carbene and an iridium complex, and show that it can be used for the asymmetric, diastereodivergent synthesis of γ-butyrolactones.
The sugar d-apiose is important in plant cell wall polysaccharides. Here the authors elucidate the complex, multistep biosynthetic pathway for its production using enzyme crystal structures and computational analysis.