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Catalysts are dynamic species, whose structure can change over the course of a reaction. Here, structural changes are mapped for cobalt–palladium nanoparticles during CO oxidation, showing a reconstruction to CoOx on palladium surfaces. Furthermore, the composition-dependent reconstruction can be correlated with the trend in catalytic activity.
One of the major routes for the use of CO2 in chemical production is the formation of carbonates via cycloaddition of CO2 to epoxides. This work uses a range of experimental and computational techniques to map out the elusive key intermediates in this process.
The electrochemical reduction of carbon dioxide allows recycling of the greenhouse gas to produce chemicals and fuels. In this Review, Seh and co-workers discuss the progress in operando techniques applied to heterogeneous carbon dioxide electroreduction, highlighting the mechanistic insights that these techniques have provided.
Two-dimensional materials have been in the spotlight since the discovery of graphene, and over time an extensive library of other ultrathin layered structures have emerged. In this Review, Pumera and Chia gather and discuss the features of this class of materials and review their recent applications in electrocatalysis.
Mupirocin is a clinically important antibiotic, but the biosynthesis of its tetrahydropyran moiety—an oxygen heterocycle essential for its bioactivity—has remained elusive. Here, Willis, Crump and co-workers report an enzymatic reaction cascade catalysing this ring formation from a non-activated C–H bond.
The function of putative bacterial vitamin K-dependent carboxylases (VKDCs) has so far been uncertain. Now, Micklefield and co-workers show that a bacterial VKDC orthologue is involved in the biosynthesis of the antibiotic malonomycin, generating an unusual malonic acid moiety that is essential for its biological activity.
Indirect methods are generally adopted to elucidate complicated mechanisms of transition metal catalysis. Now, a way to directly observe transient manganese species and monitor key reaction steps has been established by using time-resolved multiple-probe spectroscopy.
Models play a significant role in the development of catalysts. However, they are constructed using a reductionist approach and this poses the question of their relevance for the comprehension of physical phenomenon.
Despite being used as a water-oxidation catalyst in alkaline electrolysis for over a century, the details of how Ni–Fe (oxy)hydroxide catalysts function remains unclear. Now, using a nanoparticle model system, the intrinsic activity and underlying catalytic mechanism is probed.
The mechanism of methanol coupling to methyl formate over single-crystal gold catalysts has been firmly established but barely reconciled with experiments performed under practical conditions. Now, a method to close this gap has been reported, which enables the prediction of the reaction´s selectivity for a broad range of experimental conditions.
The nature of the active sites of molybdenum trioxide and molybdenum carbide, two related catalysts with great potential for hydrodeoxygenation reactions, is still under debate. Now, a comparative operando near-ambient-pressure XPS study during hydrodeoxygenation of anisole reveals important differences between these two materials.
Methanol synthesis from methane is a promising route to valorize this abundant natural gas, but existing thermal processes require harsh reaction conditions. Now, a photocatalytic approach based on TiO2-supported iron oxide species is described, which affords methanol in high yield and selectivity at ambient conditions.
Catalytic studies on single crystals are very insightful, but it is often difficult to extend their conclusions to an actual catalytic process due to gaps in the experimental conditions. Now, Madix and co-workers report a method to bridge these gaps using the oxidative coupling of methanol on gold as an example.
The reason for the high water-oxidation activity of Ni(Fe)OxHy catalysts in alkaline electrolyte is not yet well understood. Now, Chorkendorff and co-workers report that oxygen evolution is limited to the near-surface region by measuring the activity trends of mass-selected NiFe nanoparticles.
The production of higher alcohols is very valuable because of their high volumetric energy density. Now, Sargent, Sinton and co-workers report the design of copper nanoparticles with tailored nanocavities that promote n-propanol formation by the coupling of C2 and C1 intermediates inside the cavity.
Manganese carbonyl complexes are promising electrocatalysts for CO2 reduction, but the intricate mechanisms are difficult to probe. Here, vibrational sum-frequency generation spectroscopy is used to detect the transient catalytic intermediates, providing experimental evidence for the mechanism and demonstrating the utility of the analytical approach for molecular electrocatalytic processes in general.