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Ethylene oxide is a key platform chemical that is produced industrially from the epoxidation of ethylene on silver catalysts, but the precise mechanism remains elusive. Now, in a joint computational–experimental effort, a phase of the silver catalyst grown on (100) facets that contains square-pyramidal subsurface oxygens and is stabilized by strongly adsorbed ethylene is identified as the active phase, and the mechanism is revealed.
Nanoparticles are often stabilized by capping ligands but the specific role of such ligands during catalytic processes is often ignored. Now, in situ techniques including spatially resolved infrared nanospectroscopy reveal the ligand-assisted formation of a catalytic microenvironment on the surface of silver nanoparticles with nanoscale precision during CO2 electroreduction.
Unstrained aryl–aryl bonds are among the most inert bonds in organic chemistry. Now the development of a split cross-coupling strategy enables the direct functionalization of such bonds through Rh-catalysed C–C cleavage and cross-coupling with aryl halides, providing a method for biaryl synthesis.
The synthesis of well-defined heterostructure interfaces can be leveraged to design advanced catalysts. Now a catalyst consisting of carbon-supported Janus particles with crystalline Ru and amorphous CrOx sides is shown to achieve high performance for both alkaline hydrogen oxidation and evolution reactions due to the synergy between both sides.
In 2018 a descriptor was put forward to correlate the activity of various electrocatalytic reactions on carbon-based single-atom catalysts, but some data the work was based on were later found to be incorrect. This work revisits and amends the original 2018 study while presenting a modified version of the φ descriptor.
Catalytic conjunctive cross-coupling for the generation of densely functionalized sp3-rich scaffolds that are often found in biologically active compounds is underdeveloped. Now, iron-catalysed dicarbofunctionalization of olefins with dialkylzinc and haloalkanes provides access to synthetically challenging C(sp3)-rich molecules.
Mucins are glycosylated proteins with important biological functions such as protection. Although glycopeptidases can cleave them, dedicated hydrolytic enzymes specific for mucins were unknown. Now microbial mucinases are discovered that specifically recognize mucin O-glycan clusters and employ two glutamic acid residues for catalytic cleavage.
The reasons for epistasis, wherein mutations interact non-additively, are often not fully understood. Now it is found that shifting the rate-limiting step from substrate binding to the chemical reaction step during the directed evolution of β-lactamase correlates with epistasis.
[Cu(phen)(binap)]+ features a relatively high photocatalytic activity, but its low photostability hinders its use in organic chemistry. Now immobilization of this motif on a metal–organic framework matrix enhances its stability and excited-state lifetime, enabling the promotion of [2+2] cycloadditions of styrenes with a variety of olefins, including electron-deficient alkenes.
Electrochemical cross-electrophile coupling with alkyl halides for the construction of C(sp3)–C(sp3) bonds is generally limited to activated alkyl halides. Now this approach is extended to coupling of unactivated alkyl halides using a nickel catalyst under mild conditions.
The direct cross-electrophile coupling of (hetero)aryl halides and pseudohalides is challenging. Now this reaction is facilitated by a visible light-induced palladium catalytic system that differentiates the reactants on the basis of the bond dissociation enthalpy affording unsymmetrical (hetero)biaryls.
S-formyl thiols can be produced by S-formylation reactions in enzymatic processes that fix CO2 through the formate dehydrogenase enzyme. Here the authors show the use of an organocatalytic metal-free process for the direct mono- and di-S-formylation of thiols using CO2.
Multiple parameters are generally responsible for the reactivity of particulate catalysts, although nanoparticle proximity is often neglected. Here the authors report the impact of such structural factor using the hydrogenation of benzaldehyde over PdAu nanoparticles supported on macroporous SiO2 as the probe reaction.
Photocatalytic H2O2 production from water and air is limited by the availability of these substrates and charge carriers at the catalytic sites. Here a donor–acceptor covalent organic framework acts as a supply chain for the delivery of charge, water and oxygen, resulting in 17.5% quantum efficiency under visible light irradiation.
C–H activation in organic chemistry usually relies on precious and toxic transition metals. Now it is reported that a sustainable photo-promoted iron-catalysed aromatic imine C–H alkenylation reaction with alkynes circumvents previous limitations of related iron-catalysed reactions that required additives or high reaction temperatures.
Chemoenzymatic cascade reactions are often hindered by catalyst incompatibility. Now, the co-packing of catalyst-loaded Pickering emulsion droplets and solid microspheres into a continuous-flow column reactor leads to efficient combination of homogeneous, heterogeneous and enzymatic catalysts.
Acetyl-CoA carboxylation is the canonical route for endogenous malonyl-CoA formation in cells. Here, the authors design a non-carboxylative malonyl-CoA pathway independent of acetyl-CoA into multiple microbes for efficient malonyl-CoA-derived natural products biosynthesis.
The mechanism by which bimetallic catalysts can outperform their monometallic counterparts is often unexplained. Now nitrate hydrogenation on bimetallic catalysts is shown to proceed via the electrochemical coupling of hydrogen oxidation and nitrate reduction half-reactions, each of which occurs on one metal component.
Axial chirality is a key element in many valuable compounds, such as ligands in organic chemistry or pharmaceuticals. Now the catalytic atroposelective synthesis of acyclic 1,3-dienes by chiral phosphoric acid-catalysed bromination is described, expanding the chemical space of axially chiral compounds.
Precious-metal-free catalysts for water oxidation commonly suffer from low stability in acidic electrolytes. Now, by controlling the intergrowth of the γ-MnO2 structure, it has been possible to achieve 2 A cm−2 at 2 V and a stability of over 1,000 hours at 200 mA cm−2 in a polymer electrolyte membrane electrolyser.