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Achieving high enantioselective control in the hydrogenation of aliphatic ketones is a long-standing challenge. Now, the design of a spiro iridium catalyst with a narrow, crowded chiral pocket allows highly enantioselective hydrogenation of these compounds.
Tuning the structures of subnanometric metal clusters is challenging but can unlock unexpected catalytic properties. Here, the authors show that changing the composition of MFI zeolite-encapsulated PtSn subnanometric clusters by adding just a few tin atoms can lead to a remarkable stability enhancement in propane dehydrogenation.
Polyketide biosynthesis has remained exclusively based on polyketide synthases. Now, it is shown that certain thiolases can be employed instead, providing a method that offers distinct advantages for the synthesis of valuable products.
Spinel oxides have attracted interest as water oxidation catalysts due to their efficiency and cost-effectiveness. Now, the covalency competition between tetrahedral and octahedral sites is shown to dominate the OER activity on spinel oxides, and the design principle is used to predict and confirm the superior activity of [Mn]T[Al0.5Mn1.5]OO4.
The cleavage of C–F bonds through hydrodefluorination is challenging and has been traditionally limited to unsaturated fluorocarbons. Now, a simple plasmonic approach based on the use of aluminium nanocrystal-supported palladium nanoparticles is introduced to effectively upgrade fluoromethane under visible light.
Site-selective functionalization at chemically inert positions within hydrocarbon molecules is a major challenge in organic chemistry. Iron-catalysed borylation at less-reactive positions vicinal to common functional units by sequential isomerization/protoboration of alkenes is reported.
The asymmetric O-alkylation of alcohols is a useful route to chiral ethers, but aliphatic secondary alcohols have proven to be difficult substrates. Here the authors report a method to achieve this by developing conditions to avoid the decomposition of the alkylating agent.
Methods for the enantioconvergent tertiary C–H functionalization are scarce, but desired for the construction of valuable compounds. Now, a highly enantioconvergent tertiary β-C(sp3)–H amination of racemic ketones with copper/chiral phosphoric acid dual catalysis is reported.
The biogenesis and stereochemical origin of many natural products remain unknown. Now the biosynthetic pathway of brevianamide A is elucidated. An isomerase is discovered that can catalyse pinacol rearrangement without a cofactor and determine the stereochemistry of the bicyclo[2.2.2]diazaoctane ring.
Metal–support interactions can effectively modify the catalytic properties of heterogeneous composites. Here, the authors report the possibility of controlling the interaction between cobalt and a ceria–zirconia support by changing the particle size of the latter, resulting in a superior CO2 hydrogenation system.
Understanding the nature of active sites is central to controlling the activity of a given catalyst. This work combines operando characterization and computational techniques to examine the oxygen evolution reaction mechanism on RuO2 surfaces.
Photoswitching of stereochemistry opens up the possibility of controlling the selectivity of catalytic reactions in a non-invasive manner. Here the authors report a set of phosphoramidite-based molecular switches that allow reversible switching of chirality—and hence tuning of catalytic performance—even as competing pairs of chiral catalysts.
Penicillin-binding protein-type thiosterases are recently discovered trans-acting enzymes constructing macrocycles during non-ribosomal peptide biosynthesis. Now, their synthetic potential is explored and a protein crystal structure provides insights into their unusual stereochemical requirement.
Non-polar gaseous reactants such as N2 and H2 exhibit low solubility and slow transport in non-aqueous solvents and conventional gas diffusion electrodes cannot avoid non-aqueous electrolyte penetration. Here, transport limitations and catalyst flooding in tetrahydrofuran are overcome by using a stainless steel cloth-based support for lithium-mediated ammonia synthesis paired with H2 oxidation.
Efficient hydrogen oxidation catalysts must maintain an oxide-free metal surface in a relatively high potential range. Now, a catalyst consisting of Ru clusters partially confined in the lattice of urchin-like TiO2 crystals is shown to catalyse the reaction up to a potential of 0.9 VRHE with high mass activity and CO tolerance under both acidic and basic conditions.
Electrocatalytic reduction of CO2 into multicarbon (C2+) products is a highly attractive route for CO2 utilization. Now, a fluorine-modified copper catalyst is shown to achieve current densities of 1.6 A cm−2 with a C2+ Faradaic efficiency of 80% for electrocatalytic CO2 reduction in a flow cell.
There has been a long-standing debate on whether heterogeneously catalysed Suzuki cross-couplings can occur homogeneously due to metal leaching. Here the authors show that while the palladium from the nanoparticle catalyst is mobile during the reaction, the active sites remain heterogeneous in nature.
Oxidative carbonylation using CO/O2 is an attractive strategy to construct carbonyl compounds, but the explosive limit of the gas mixture hampers its application. Now, this safety issue is overcome in the aminocarbonylation of alkynes by replacing the external oxidant O2 by electrochemistry facilitating a mild and safe reaction.
Palladium-catalysed allylic substitution is a widely used method in organic synthesis, although it requires prefunctionalized starting materials or stoichiometric oxidants. Here the authors report a radical route to form π-allylpalladium complexes, and develop a 1,4-aminoalkylation of dienes under redox-neutral conditions.
Reducible metal oxides selectively catalyse the hydrodeoxygenation of C–O bonds in bio-based aromatic molecules, although they show limited performance. Now, using TiO2 as an example, a method is reported to enhance the activity of the oxide by surface doping with an ultralow loading of Pt.