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Controlling the selectivity of electrocatalysed C–H activation with earth-abundant base metals can increase its synthetic impact. Now chemodivergence of an electrocatalysed enantioselective C–H activation is achieved by using either ligand-bound Ni or Co in the catalytic system.
Electrosynthesis of n-propanol from CO has been limited by poor selectivity and low product concentration. Here a Sn–Cu catalyst/carbon/ionomer heterojunction is prepared where the adjacent atomic active sites favour the coupling of C1 and C2 intermediates to C3 product with 47% Faradaic efficiency and the reversal of electro-osmotic drag concentrates the product to 30 wt%.
Hydrogenation and oxidation, common reactions in organic synthesis, usually require hydrogen or oxygen donors. Now, a study reports a hydrogenative oxidation protocol that allows N-heteroarenes to be converted to lactams, with water providing both the reducing hydrogen and oxidizing oxygen.
Efficient charge carrier separation is a substantial roadblock to achieving high performance in photoelectrochemical systems based on transition-metal oxides. Here a metal vacancy strategy is used to enhance hole mobility, resulting in general enhancement of photocurrent density in WO3, TiO2 and Bi2O3 photoanodes.
Ru and Ba are common partners within ammonia synthesis catalysts, but the mechanism by which the base promotes the metal is not fully understood. Here the use of conductive carbon supports reveals intriguing mechanistic aspects of this promotion effect and enables the generation of an advanced ammonia synthesis catalyst.
Despite the existence of many N–N-containing natural metabolites, little is known about the enzymatic mechanisms of N–N bond formation. Now, a catalytically relevant X-ray crystal structure of an N–N-bond-forming enzyme, PipS, is reported and detailed insights into its catalytic mechanism are provided.
The catalytic enantioconvergent nucleophilic fluorination of alkyl halides using inexpensive alkali metal fluorides is a persistent challenge. Now this has been achieved by synergistic hydrogen bonding phase-transfer catalysis combining a chiral bis-urea hydrogen bond donor and an onium salt.
In situ profiling of lysosomal proteomes is impeded by the acidic and digestive environment of lysosomes. Now, a bioorthogonal photocatalytic system (CAT-Lyso) is developed that is compatible with these conditions, enabling the proximity labelling of lysosomal proteomes within living cells.
Medium- and branched-chain diols and amino alcohols are important industrial feedstocks, but they are biosynthetically challenging to produce. Here the authors introduce a modular polyketide synthase platform for the efficient production of these compounds.
Allenes are versatile substrates in synthetic chemistry. Now an iron catalyst enables unusual regioselectivity by mediating an electrophilicity reversal of allenes for stereoselective alkenylzincation reactions affording 1,4-diene zinc products.
Co–Mn spinel oxides are the most promising precious-metal-free catalysts for oxygen reduction in alkaline electrolytes, but their structure–activity properties are not yet fully understood. Now, in situ XRD and REXS performed on MnCo2O4 identify surface tensile strain at low potentials and a reversible transformation between cubic and tetragonal structures.
High-throughput computational screening of multicomponent molecular photocatalytic systems offers a strategy to minimize the screening of large numbers of photosensitizer–catalyst combinations. Here a machine learning-accelerated approach using multiple descriptors shows strong predictive power in experimentally validated systems for CO2 reduction.
Iminium-catalysed cycloaddition is a prominent example of organocatalytic reactivity, yet a biological counterpart has not been identified. Now, the authors report biochemical, structural and computational evidence for iminium catalysis by the natural Diels–Alderase SdnG.
Monitoring the temperature of a catalyst’s active site during reactions can offer important insights into reactivity, but broadly applicable methods are lacking. Here the authors evaluate the potential of extended X-ray absorption fine-structure thermometry to observe variations in the temperature of nickel nanoparticles throughout representative gas–solid reactions.
Hydrocarbon selectivity in photoelectrochemical CO2 reduction has been limited due to a lack of low-overpotential catalysts and high-photovoltage semiconductors. Here Cu nanoflowers are interfaced with perovskite light absorbers for bias-free conversion of CO2 to ethane and ethylene coupled to water or glycerol oxidation.
The behaviour of nanoconfined water can be very different from that of the bulk and is challenging to understand at a molecular level. Now, molecular simulations and kinetic experiments provide insight into the increased activity of hydronium ions in water nanoconfined within zeolite pores.