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Ribozymes that use the cellular cofactor S-adenosyl-l-methionine to methylate RNA remained elusive. Now, such a ribozyme is reported by identifying natural sequences that are active in vitro; and crystal structures of the ribozyme with and without the cofactor are determined.
Enantioselective C(sp3)–C(sp3) coupling plays an important role in organic synthesis, but limitations remain. Now, cobalt-catalysed enantioselective C(sp3)–C(sp3) coupling between achiral fluoroalkenes and alkyl halides enables the streamlined and auxiliary-free synthesis of chiral fluoroalkanes.
The challenge in non-oxidative coupling of methane lies in the activation of the first C–H bond while avoiding further dehydrogenations, which lead to the formation of coke. Here, atomically thin platinum nanolayers on two-dimensional molybdenum titanium carbides are reported as a superior catalyst for this reaction owing to reduced coke formation.
The valorization of CO2 via its hydrogenation to methanol is a highly sought-after reaction although only a handful of catalysts can efficiently promote this transformation. Here, the authors engineer the interface of a copper catalyst supported on a silica–molybdenum MXene composite, achieving a remarkable performance in the reduction of CO2 to methanol.
Periselective catalytic asymmetric cross-Diels–Alder reactions between two different conjugated dienes remain underdeveloped. Now, the selectivity challenges are overcome in such a reaction of electron-poor 2-pyrones and unactivated conjugated dienes, and an ambimodal transition state is identified.
Despite its importance in the context of natural gas engines emissions treatment, methane oxidation remains challenging. Now, the authors introduce an approach to stabilize PdOx rafts on ceria by trapping Pt single atoms in the support resulting in a superior catalyst for this transformation.
Chemoselective reactions are often characterized by an activity–selectivity trade-off that renders their optimization difficult. Here gold nanoparticles equipped with a platinum monolayer are introduced that, thanks to lattice expansion and ligand effect, achieve a remarkable performance for the chemoselective hydrogenation of halonitrobenzenes
Establishing structure–activity relationships is crucial for the design of improved catalysts. Now, by developing a method based on electrochemical scanning tunnelling microscopy, the active sites of graphene/iron/platinum interfaces are visualized with atomic-scale precision in real time during the hydrogen evolution reaction.
Reductive aminases show strong potential for the sustainable synthesis of chiral amines, but their application in industrial scale processes is lacking. Now, such an enzyme is screened and engineered allowing its use in commercial manufacturing of abrocitinib JAK1 inhibitor in multi-metric tons.
Solvent structuring affects the energy landscape of catalytic reactions, but the quantitative understanding of such effects remains difficult. Now, the structure of water within the micropores of different zeolites is disclosed together with the effects that its reorganization has over alkene epoxidation catalysis.
Information on how metabolic networks respond to the utilization of a non-natural carbon source remains scarce. Now, yeast’s response and adaption to xylose as an alternative carbon source is investigated; cell engineering enhanced growth provides an improved platform to produce chemicals from xylose.
The design of artificial organelles for applications in living cells faces several challenges such as cellular uptake, stability and biocompatibility. Now, fusion of exosomes creates beneficial nanoreactors and their use for compartmentalized biocatalytic cascade reactions in cells is demonstrated.
The mechanism of heterogeneous aqueous-phase aerobic oxidations remains under debate. Now, it has been shown that the reaction can be described as two coupled electrochemical half-reactions for oxygen reduction and substrate oxidation, and the thermochemical rates can be derived from the electrochemical half-reactions via the application of mixed potential theory.
Understanding the role of hydrogen bonds at the electrode interface is important for controlling the kinetics of the oxygen-reduction reaction. Here the authors modify gold and platinum surfaces with a series of protic ionic liquids to show that pKa can be used to optimize proton-coupled electron transfer through hydrogen bonding.
CH4 selectivity in CO2 photoreduction is a kinetic challenge as a result of the complex pathway involving many intermediates. Here, the authors present dual-metal-site pairs embedded in a metal-organic framework structure with flexible adaptive active sites leading to high CH4 activity and selectivity.
Modifying Pt surfaces with highly oxophilic metals can increase the hydrogen evolution and oxidation performance in alkaline media, but the underlying mechanism remains elusive. Now, it is demonstrated that the activity improvement of Ru-modified Pt mainly originates from the strain and electronic effects rather than an alternative bifunctional mechanism.
Photoelectrochemical systems based on haematite photoanodes have mainly been explored in the context of solar fuels, but their synthetic utility remain largely unexplored. Here α-Fe2O3 is employed as a catalyst for the oxidation of different organic compounds and inorganic anions using water as the oxidant in a photoelectrochemical cell.
Stereochemical control in the asymmetric dihalogenation of alkenes and alkynes is challenging. Now, an organocatalytic method is developed, whereby installing a urea-directing moiety on these substrates enables their stereo- and regioselective homo- and hetero-dihalogenation.
Common native functional groups would be appealing as handles to enable C–H annulation with diverse aromatic rings. Now, this is achieved using ketones as unconventional alkyl radical precursors providing a practical method to synthesize biologically important fused-ring systems.
Dual catalysis is widely employed by natural metalloenzymes to functionalize challenging substrates. Now, this concept is applied to artificial metalloenzymes by designing a hydroaminase with two biotinylated gold cofactors enabling an unnatural σ,π-activation mechanism of terminal alkynes.