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Formate dehydrogenase is immobilized on a scanning tunnelling microscope tip to measure the kinetic turnover of its enzymatic reaction showing that the bound NADH directly converts to NAD+ via in situ hydride exchange.
The ability to maximize electron utilization in electrosynthesis has been a long-standing goal, with research typically focusing on catalyst design or pairing disparate reactions. Now, electrocatalytic hydrogenation is performed with Faradaic efficiencies approaching 200% by producing hydrogen atoms from both the reduction and oxidation reactions simultaneously.
Electron transfer processes are almost ubiquitous, yet hard to understand thoroughly due to the variability of catalytic species involved. Now, a detailed mechanistic picture of the electron transfer associated with polypyridine nickel systems has been reported, offering an answer to the electron transfer puzzle of these complexes.
Microporous zeolites have pores of molecular dimension that can stabilize desired chemical pathways but may also introduce mass-transfer limitations. Now, synthesis protocols allow for greater control of catalyst active-site location via elemental zoning, enabling an alternative strategy to reduce mass-transfer limitations and consequently improve catalyst performance for methanol-to-hydrocarbon reactions.
Large-scale deployment of electrocatalytic hydrogenations using water as a hydrogen source is hampered by poor solubility and difficult product separation. Here the authors propose a dual hydrogenation approach, with palladium membranes used as both anode and cathode, to produce hydrogen—enabled at the anode by the low-potential oxidation of formaldehyde—that permeates to adjacent chemical compartments, where the hydrogenation of organic substrates occur.
Oxygen reduction to hydrogen peroxide is a promising alternative to replace the energy-intensive anthraquinone process in industry. Now, the hydrogen peroxide electrosynthesis performance of a carbon-supported cobalt phthalocyanine catalyst is tuned via the introduction of oxygen functional groups to the support, which optimize the electronic structure of cobalt active sites.
Polypyridine-ligated nickel complexes can mediate a variety of cross-coupling reactions. However, some mechanistic details remain poorly understood. Now, it is demonstrated that the nature of the anionic ligand strongly influences key electron-transfer events in these complexes during elementary reaction steps.
To overcome mass transport limitations in zeolite-catalysed reactions, scientists must often resort to hierarchical or nanosized zeolites; however, the synthesis of such materials remains challenging. Here the authors disclose a one-pot method for the preparation of Si-zoned MFI-type catalysts with improved diffusion properties for the methanol-to hydrocarbon reaction.
The catalytic cycle of formate dehydrogenase is generally assumed to involve an apoenzyme state according to the Theorell–Chance mechanism. Now, based on single-molecule experiments and multiscale simulations of formate dehydrogenase from Candida boidinii, an alternative mechanism that bypasses the apoenzyme state is proposed.
The dynamic transformation of Cu ions during the selective catalytic reduction of NOx on Cu zeolites is well documented, although the function of the zeolite framework has not been fully understood. Here the authors unravel the role of anionic Al sites in the zeolite framework in regulating the mobility and reactivity of Cu cations during catalysis.