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Although mechanistic understanding can drive new reactivity development, the key bond-forming and -breaking steps in catalytic cycles are often sufficiently fast to elude observation. Here, the authors photochemically produce a key intermediate in Mn-catalysed C–H functionalization, and follow the subsequent steps—spanning processes occurring over seven orders of magnitude in time—using time-resolved infrared spectroscopy.
The precise understanding of the active phase under reaction conditions at the molecular level is crucial for the design of improved catalysts. Now, Strasser, Jones and colleagues correlate the high activity of IrNi@IrOx core–shell nanoparticles with the amount of lattice vacancies produced by the nickel leaching process that takes place before and during water oxidation, and elucidate the underlying structural-electronic effects.
Due to its ready availability and low cost, copper is an attractive metal for the homogeneous reduction of CO2 to formate. However, although CO2 can readily insert into copper hydrides to produce metal-bound formate, subsequent regeneration of the catalytic species with H2 is more challenging. Here a dual strategy is used, whereby a copper hydride activates CO2 and a Lewis pair heterolytically splits H2, leading to dramatically improved performance.
Lignin-first approaches, which prioritize lignin upgrade over cellulose, can open the way to full biomass valorization, but are still hampered by the need of harsh reaction conditions and difficulties in catalyst recovery. Now, a photocatalytic strategy based on the use of cadmium sulfide quantum dots is reported that overcomes these limitations.
Post-synthesis refining of Fischer–Tropsch products is a costly but necessary step to adjust the selectivity of the process towards specific fuels. Now, a catalytic system based on a cobalt-loaded Y-type zeolite is reported that can be tuned to selectively produce gasoline, jet fuel or diesel fuel directly from syngas.
Heterogeneous photocatalysts are rarely employed in industry for the synthesis of commodity chemicals due to efficiency problems. Now, a photochromic Bi2WO6–x/amorphous-BiOCl composite is reported, which features a remarkable activity for the photocatalytic oxidation of toluene into benzaldehyde and benzoic acid.
In this Editorial, we discuss recent advances and challenges in the field of biocatalysis and introduce some relevant work you will find in this issue of Nature Catalysis.
This year marks a century since the pioneering work leading to what is now known as the Rosenmund reduction. We celebrate this landmark, reflecting upon the evolution of synthetic methodologies for reductive aldehyde synthesis from carboxylic acid derivatives and highlighting modern, improved strategies.
Artificial metalloenzymes generally consist of a synthetic (organo)metallic catalyst incorporated into a protein. Asymmetric catalysis by such metalloenzymes could result by virtue of the chiral protein environment. Now, redox-sensitive anchoring enables reversible incorporation of an iridium catalyst for transfer hydrogenation.
Typically, catalysts are discovered through trial and error coupled with chemical intuition. Now, an automatic machine-learning framework has been developed that can guide itself to find intermetallic surfaces with desired catalytic properties.
The design of new catalysts for electrochemical energy storage is of utmost importance. Here, an automated computational screening method is used to identify over 100 intermetallic surfaces as efficient electrocatalysts for CO2 reduction and H2 evolution.
Plasmonic catalysis has recently revolutionized the field of catalysis, promising to achieve improved control over catalytic reactions by targeting specific electronic excitations. In this Review, Linic and co-workers discuss the recent advances in the field, focusing on the underlying physical mechanisms and their application in catalysis, as well as limitations and future perspectives.
Knowledge of the active sites in catalysts—including the sites that form under working conditions—is vital for future design and development. Here, the authors track the atomic-scale changes in a series of well-defined cobalt-based oxide electrocatalysts, showing that the structurally distinct catalysts develop a similar structural motif as they transform into the catalytically active state.
The general importance of electrostatic effects on catalysis is well appreciated, but their use in catalyst design is both promising and challenging. This Perspective discusses recent progress and future directions towards computational optimization of biological and chemical catalysis in terms of electric fields and their connections to experimental catalytic systems.
Despite its potential, the visible light-triggered photocatalytic oxidation of toluene remains difficult due to the lack of efficient and scalable catalytic strategies. Now, a photochromic Bi2WO6–x/amorphous BiOCl composite is reported with the ability to oxidize toluene into benzaldehyde and benzoic acid with outstanding rates and quantum efficiencies.
Ta3N5 is a semiconductor with very promising photocatalytic properties. However, performing overall water splitting with this material has remained elusive. Now, Domen and co-workers report a method for the synthesis of defect-free single-crystal Ta3N5 nanorods capable of splitting water into hydrogen and oxygen in the presence of a co-catalyst.