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Directed evolution typically requires extensive screening. This work presents an ultrahigh-throughput microfluidic assay, based on a coupled reaction and fluorescence-activated droplet sorting, enabling a 960-fold activity improvement of an amine oxidase for a non-natural substrate in a single round.
Here the enantioselective lithiation of Boc-1,3-oxazinanes is reported. Transmetallation to zinc allows for regiodivergent functionalization at either C4 or C5 positions via a ligand-controlled Negishi coupling, and subsequent oxidative cleavage gives easy access to both β2- and β3-amino acids.
One of the major challenges in C–H functionalization is to achieve selectivity when multiple bonds of similar reactivity are present. Now, a method to selectively amidate sterically and electronically similar β- or γ-C–H bonds that utilize different silver catalysts is reported, giving access to valuable 1,2- and 1,3-aminoalcohols.
Targeted therapy is an important approach to reduce the side effects of medicinal drugs. This work reports the synthesis of catalytically active Pd nanostructures in exosomes that selectively target cancer cells for drug activation using biorthogonal chemistry.
Cu2O is a promising photocatalyst, although its stability is compromised by a disproportionation reaction that leads to the formation of Cu and CuO. Now, a method is reported to stabilize Cu2O nanocubes, rendering them highly active and stable for the photocatalytic reverse water–gas shift reaction.
Elucidating reaction mechanisms on electrode surfaces is of utmost importance. Now, using canonical transition state theory, Cuk and colleagues show the competing pathways by which the charge-trapping intermediates of the water oxidation reaction on n-SrTiO3 decay towards the next step in the reaction.
α-Branched amines are commonplace in pharmaceutical agents. This work reports the synthesis of α-branched amines by simultaneous C–C and C–N bond formation at the sp3 carbon branch site through an 1,1-alkene addition pathway and utilization of three readily accessible starting inputs in a single catalytic cycle.
Traditional modes of catalyst deactivation such as Ostwald ripening and particle migration and coalescence eventually lead to sintering and particle growth. Now, Cargnello and colleagues identify loading-dependent particle decomposition into single atoms as an important deactivation mechanism during methane combustion on colloidal Pd nanocrystals.
Performing photocatalytic CO2 reduction in a selective fashion with molecular catalysts represents a considerable challenge. Here, a binuclear cobalt complex featuring a bi-quaterpyridine ligand is developed that can selectively afford either carbon monoxide or formate by selection of the reaction medium acidity.
C-aryl glycosides are present in many natural products and of interest in drug design, but their chemical synthesis is challenging. This work reports an efficient and diastereoselective ortho-directed C−H glycosylation of arenes and heteroarenes with glycosyl chloride using a palladium catalyst.
Encapsulation is an effective strategy to tune metal-catalysed reactions, although its potential has not been fully explored. Here, design principles and advanced understanding of the reactivity of different polymer-encapsulated Pd nanocrystals are provided using CO oxidation as a benchmark reaction.
The development of efficient and low-cost electrocatalysts for the oxygen evolution reaction is critical for improving the efficiency of water electrolysis. Here, the inactive spinel CoAl2O4 is activated via iron substitution to achieve high activity and stability for water oxidation.
The direct amination of alcohols with ammonia is a modern and clean route for the synthesis of amines. This joint theoretical and experimental study reveals the key factors governing the activity and selectivity to primary amines on metals, which are then used for the rational design of bimetallic catalysts.
Efforts to harness the cellulolytic activity of enzyme assemblies have been mainly empirical due to the lack of quantification tools. Now this work reports experimental and theoretical approaches to quantify enzyme assemblies, revealing the parameters that are important for cellulolytic activity.
A strategy using pressure was devised to structurally identify conformational transitions in protein ensembles, allowing the rational prediction of mutations that induce pressure-driven enzyme activation. These results highlight the power of flexibility–function analyses in protein engineering design and applications.