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Simultaneously expanding the scope of electrophiles and nucleophiles for hydroamination reactions catalysed by ammonia lyases is a formidable challenge that requires a thorough reconstruction of the protein’s active site. Here, Cui et al. use a mechanism-based computational strategy to redesign the enzyme, generating a versatile hydroamination biocatalyst for C–N bond formation and demonstrating its synthetic value in the preparation of a wide range of aliphatic, aromatic and charged non-natural amino acids.
Creating enzymes with new capabilities is a key goal for synthetic biology and sustainable chemistry. Now, computational approaches have been used to quickly achieve leaps in enzyme function, providing a versatile platform for biocatalytic hydroamination.
The challenge in synthesizing hydrogen peroxide from O2 and H2O is to balance several concurrent reactions. Now, selective H2O2 production is achieved on a noble-metal-free photocatalyst based on carbon-nitride-supported antimony single atoms.
N-Heterocyclic carbenes are versatile ligands that can be used to modulate the properties of metallic surfaces. This Review focuses on efforts to tune the reactivity of metal-based heterogeneous catalysts by such molecular species, providing an overview of the techniques to study carbene–surface interaction and examples of successful catalytic reactions based on this approach.
Ammonia lyases are powerful catalysts to access C–N bond formation via hydroamination, but show a narrow synthetic scope. Now, by computational redesign of an aspartase, a C–N lyase is developed that shows cross-compatibility of non-native nucleophiles and electrophiles expanding the synthetic scope.
Hydrogen peroxide is an interesting target for artificial photosynthesis, although its actual production via the two-electron oxygen reduction reaction remains limited. Now, a carbon nitride-supported antimony single atom photocatalyst has been developed with a superior performance for this process.
C−H bond functionalization methodologies usually rely on substrate-controlled directing-group chemistries to facilitate regioselective activation. Now, chemobiocatalytic cascades are reported that enable catalyst-controlled regioselective access to aryl nitriles, primary amides and carboxylic acids.
Improving the efficiency of carbon yield in heterotrophic microorganisms is desired for biomanufacturing. Now, a product-independent and energy-efficient CO2 sequestration system that maximizes carbon conversion has been developed, as showcased by the production of chemicals reaching their theoretical yields.
Nanozymes can provide cost and stability advantages over natural enzymes, but they usually display low catalytic activity and inferior kinetics. Now, a highly active nanozyme is developed that shows comparable kinetics to horseradish peroxidase in the oxidation of a commonly used artificial substrate.
The strong metal–support interaction is an important phenomenon for the modulation of a catalyst´s performance but is traditionally restricted to reducible oxide supports. Here, a CO2-induced strong metal–support interaction is reported for gold nanoparticles supported on non-reducible MgO to yield a superior oxidation catalyst.
In the face of global plastic pollution, enzymatic degradation of poly(ethylene terephthalate) (PET) has attracted much attention. Now, structural and biochemical studies reveal a minimal mutational strategy to increase the activity of PET-degrading enzymes, with potential evolutionary implications.
Conductive polymers are attractive materials for the construction of photoelectrodes in the context of artificial photosynthesis, although their performance is still limited. Now, an organic semiconductor photoanode for water oxidation is presented, which provides high photocurrent density for over 30 minutes.