Browse Articles

Aqueous electroconversion of biomass derivatives to polymer precursors has been demonstrated at the laboratory scale with low yield. Here a solid polymer electrolyte reactor is engineered to limit side reactions, yielding a high rate and and a high product concentration in a 4.3-kW pilot-scale platform.

Ni-based CO₂ reduction electrocatalysts have been reported to produce multicarbon products up to C₆ but with limited selectivity. Here the reaction mechanism of the process is elucidated. Consequently, pulsed potential electrolysis and electrolyte deuteration are respectively employed to enhance the selectivity of branched hydrocarbons and increase the total hydrocarbon Faradaic efficiency to 22%.

The mechanism by which sulfur is incorporated into the furanose ring in albomycins—a group of natural nucleoside antibiotics—remains unclear. Now, this work explains how twitch radical S-adenosyl-l-methionine enzyme AbmM catalyses sulfur-for-oxygen replacement in the biosynthesis of albomycin δ₂.

Methods for deuterium labelling of C–H bonds under mild conditions are sought after. Now an electrocatalytic method for H/D exchange via a radical-mediated pathway is described, using a boron cluster as a radical shuttle during the coupling process of deuterium and carbon radicals.

Enantioselective catalytic C(sp³)–H fluorination has been limited to electrophilic fluorine sources. Now chiral palladium catalysts bearing amino sulfonamide ligands enable enantioselective incorporation of nucleophilic fluoride into unactivated aliphatic C–H bonds with demonstrated applications to ¹⁸F-radiolabelling using [¹⁸F]KF.

Reconstruction of Cu catalysts under electrochemical CO₂ reduction conditions is a well-reported phenomenon. Here the reconstruction of bimetallic Cu–X catalysts is investigated to reveal the roles of atomic miscibility and intermediate binding on surface reconstruction and the resulting effects on product selectivity.

The formation of multi-carbon products in photocatalytic CO₂ reduction has been limited by the supply of sufficient excited electrons to C–C coupling active sites. Here Cu₂ sites introduced into metal–organic frameworks with semiconductor photocatalyst-filled pores allow multi-electron transfer and improved solar efficiency towards C₂H₄.

The CO dehydrogenase–acetyl-coenzyme A synthase complex produces acetyl-coenzyme A from CO₂, but its structural dynamics during catalysis remain unresolved. Now cryo-EM maps of six intermediate states reveal how ligand binding to a Ni–Fe cluster orchestrates the conformational changes of the complex during catalysis.

Chemical synthesis of chiral β-hydroxy-α-amino acids usually requires multiple steps. Now a biomimetic enantioselective aldol reaction of glycinate and aldehydes catalysed by a chiral pyridoxal has been achieved, providing efficient access to a large number of chiral β-hydroxy-α-amino esters.

The scope of Lewis acid catalysis mediated by enzymes is low compared with the range of reactions it drives in organic synthesis. Now the substitution of the iron centre with copper, and the subsequent directed evolution, enabled a non-haem iron hydroxylase to efficiently catalyse asymmetric abiotic Conia-ene cyclizations.

The intermolecular addition of O-centred radicals to alkenes is a challenging endeavour in synthetic chemistry. Now ene-reductases are used to tame reactive O-radicals for intermolecular and enantioselective radical hydroalkoxylation involving a ground-state single-electron radical mechanism.

The electrochemical oxidation of methane is a promising process but controlling its selectivity for a partial oxidation product such as methanol is very challenging. Now a strategy to convert methane into methanol with high selectivity is demonstrated, using an IrO₂ catalyst and CO₃²⁻ in the electrolyte as the oxygen source.