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Artificial metalloenzymes can combine the scope of synthetic catalysts with the selectivity provided by the protein scaffold, but recycling of the single components is challenging. This work provides a methodology for controlling assembly and disassembly of an artificial metalloenzyme.
Multicomponent couplings allow the rapid formation of molecular complexity from simple starting materials. Now, Ellman and co-workers report a three-component coupling that proceeds via aryl or vinyl C–H addition to dienes and aldehydes, and elucidate the mechanism by isolating a catalyst-bound intermediate. The C–H addition does not occur without all three components in place.
Prenylation is a common step in the synthesis of many natural products, and enantioselective variants require the use of enzymatic catalysts. Now, You and co-workers report a palladium phosphoramidite catalyst capable of enantioselective, dearomative prenylations across a broad range of starting materials, and demonstrate its power in a number of natural product syntheses.
High activity and stability of enzyme cascades are key to their biotechnological application. Here, Willner and co-workers demonstrate that encapsulation in metal–organic framework nanoparticles can improve these features for two- and three-enzyme, as well as NAD+-dependent, cascades.
The bioenergetic metabolism of all life today depends on proton gradients; however, it remains unclear how such gradients developed in early life. Here, Mansy and co-workers establish a possible prebiotic mechanism in which iron–sulfur peptide redox networks generate a trans-membrane pH gradient.
The synthesis of complex terpene compounds in the laboratory using man-made catalysts has proven to be much more complicated than in nature. Now, Tiefenbacher and co-workers report the use of an enzyme-mimicking supramolecular catalyst for the efficient and short synthesis of tricyclic sesquiterpenes.
The synthesis of nanocatalysts with small dimensions and high surface-to-volume ratios is of great interest to lower catalyst costs and exploit catalytic performance enhancements through size effects. Now, Prinz and colleagues show that two-dimensional growth of platinum nanoparticles with suppressed thicknesses can be promoted with passivation-gas-incorporated atomic layer deposition.
Though pentamethylcyclopentadienyl rhodium(iii) complexes have been successfully employed for C–H functionalizations, stereocontrol can be difficult due to the lack of vacant coordination sites on the metal centre. Here, Yoshino, Matsunaga and co-workers show that chiral anions can be used alongside the achiral rhodium complex to catalyse C–H activation and subsequent asymmetric conjugate addition.
The efficient design of electrochemical CO2 reduction catalysts requires high CO2 concentrations on the catalyst surface. Here, Cui and co-workers make use of flexible, hydrophobic, nanoporous polyethylene membranes with good gas permeability to design a catalytic set-up that mimics the alveolus structure in mammalian lungs, achieving high activity and selectivity to CO.
A haem–carbenoid has been proposed to be involved in abiological enzymatic reactions. Now, Hilvert and co-workers provide crystallographic evidence for a haem–carbenoid intermediate as the reactive species in an olefin cyclopropanation reaction catalysed by an artificial metalloenzyme.
Methanol-to-olefins (MTO) conversion over zeolites is a promising route for the production of light olefins. Now, Corma and co-workers show that using mimics of reaction intermediates as structure-directing agents allows the synthesis of highly selective zeolite MTO-catalysts.
The preparation of functionalized amino acids from inexpensive aldehydes is challenging. This work describes the biocatalytic synthesis of l-methionine by applying gaseous CO2 pressure and a coupled amination step to drive the unfavoured equilibrium of a reverse carboxylation reaction.
Supported metal nanoparticles are indispensable catalysts in industry, yet they are often subjected to severe sintering. Now, a general method based on metal immobilization within zeolite is reported for the preparation of highly sinter-resistant catalysts for a broad range of industrially relevant processes.
The properties of polymers depend on monomer composition and chain length, but regulating these structural features during polymer synthesis is a challenge. Now Hecht and co-workers report a photoswitchable catalyst system that can repeatedly be switched between ON and OFF states, allowing remote control of the polymerization process. Furthermore, copolymerization with control over monomer incorporation is demonstrated.
Predicting metal–support combinations that can afford stable single-atom catalysts remains a complex problem. Now, a computational method is reported that can be used to screen interaction strengths between metals and supports and identify those pairs that generate strongly adsorbed single-atom catalysts.
Organic synthesis relies on the ability to convert simple starting materials into compounds with greater molecular complexity. Here, Trost and co-workers use branched aldehydes as nucleophiles for asymmetric Mannich reactions, and the products of these reactions as electrophiles for the addition of a range of carbon nucleophiles. This provides a simple, stereodivergent route to 1,3-aminoalcohols.
Electrolysis uses clean electricity to form chemical products but typical water electrolysis produces hydrogen which is hard to store oxygen which is a waste gas. Here, paired electrolysis is performed with an palladium membrane reactor to carry out two organic reactions simultaneously. The dense palladium membrane enables the two reactions to proceed in different solvents and the reaction rates and selectivities can be independently controlled.
Cross-coupling of aryl compounds is one of the most powerful carbon–carbon bond forming reactions available, and typically involves the use of expensive and scarce palladium salts. Here Bedford and co-workers show that iron can be an effective catalyst for Suzuki biaryl couplings.
The conversion of carbon dioxide into multi-carbon alcohols would enable the synthesis of sustainable liquid fuels with high energy densities. Now, vacancy-engineered core–shell copper-based catalysts are able to shift the selectivity of electrochemical CO2 reduction into alcohols instead of alkenes, as obtained with bare-copper catalysts.
The proper verification of the stability of metal oxide catalysts for water electrolysis in acid electrolyte remains unresolved. Here, the ‘stability number’ is introduced to evaluate the dissolution mechanisms of various iridium-based oxides and to facilitate benchmarking of catalysts independent of loading, surface area or involved active sites.