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The selective electrochemical conversion of ketones to value-added products still represents a challenge, due to a lack of fundamental understanding. Now, a principle has been revealed that allows the steering of the electroreduction of aliphatic ketones on platinum by carefully controlling the coordination number of the platinum atoms.
The synthesis of highly branched low molecular weight products — potential synthetic lubricants — directly from ethylene is challenging when highly efficient early transition metal catalysts are employed. Now, an alkane soluble co-catalyst permits the synthesis of such polyethylenes using a zirconium catalyst in a saturated hydrocarbon solvent, where competitive solvent coordination at the active site of the catalyst is relatively unimportant.
Photocatalytic water splitting with particulate semiconductors represents a promising strategy for the generation of hydrogen as a solar fuel. This review covers recent advances in the development of reaction systems and photocatalysts towards the scale-up of this technology, emphasizing at the same time the challenges to overcome.
While Ru-based electrocatalysts are among the most active for acidic water oxidation, they suffer from severe deactivation. Now, Yuen Wu, Wei-Xue Li and co-workers report a core–shell Ru1–Pt3Cu catalyst with surface-dispersed Ru atoms for a highly active and stable oxygen evolution reaction in acid electrolyte.
The hydrogenation of CO2 to form methane has been known for over a century. However, given increased interest in small-molecule activation for energy storage, and improved catalysts and understanding of the process, it is worthwhile to look again at the reaction. This Perspective discusses recent work on the fundamentals of the Sabatier reaction and also the potential for large-scale applications.
The electrocatalytic reduction of carbonyl groups is gaining attention in the context of biorefinery. However, fundamental knowledge on such processes is still limited. Now, the selectivity for the electroreduction of acetone on platinum single crystals is studied, revealing a remarkable structural sensitivity.
The electrochemical reduction of nitrogen to ammonia represents a challenge of major interest that would substantially decrease the burden of the energy-consuming Haber–Bosch process. Now, Yin, Yan, Zhang, Si and colleagues achieve high ammonia yield and Faradaic efficiency over 66% using bismuth nanocatalysts promoted by alkali cations.
Iron single-atom catalysts are among the most promising fuel cell cathode materials in acid electrolyte solution. Now, Shui, Xu and co-workers report concave-shaped Fe–N–C nanoparticles with increased availability of active sites and improved mass transport, meeting the US Department of Energy 2018 target for platinum-group metal-free fuel cell catalysts.
The electrochemical reduction of carbon dioxide to fuels and feedstocks has received increased attention over the past few years. In this Review, Roldan Cuenya and co-workers discuss strategies to achieve high selectivity towards multicarbon products via rational catalyst and electrolyte design.
Metal oxides have been identified as a promising class of catalysts for carbon–oxygen bond cleavage in the context of biomass valorization, although the systematic understanding of their reactivity remains elusive. Now, a combination of catalytic screening and first principles calculations provide important insights into this family of catalysts.
Photoelectrochemical cells have been widely used for the production of solar fuels, but have seen limited applications in organic synthesis. Here the authors demonstrate photoelectrocatalytic C–H amination of aromatics, using haematite as the photoanode.
Copper on ceria is an excellent catalyst for the low-temperature water–gas shift reaction. Here the active sites are directly imaged by electron microscopy and probed with in situ spectroscopy, showing that the reaction proceeds via a cooperative mechanism whereby the Cu+ chemically adsorbs CO while an adjacent Ov–Ce3+ site dissociatively activates H2O.
Chiral γ-lactams are of significant interest being present in numerous pharmaceutical agents; however, their chemical synthesis is complex, requiring pre-functionalized starting materials. Now, Park and Chang report an iridium-based catalyst system for the production of chiral γ-lactams from an abundant feedstock via an intramolecular asymmetric sp3 C−H amidation.
Low-molecular-weight, highly branched polyethylenes are attractive candidates for synthetic lubricants, but their efficient production is constrained by a lack of effective catalytic methods. While conventional group IV transition metal catalysts produce diverse polyethylenes on a huge scale, they are unable to produce highly branched polyethylenes. Here a hydrocarbon-soluble organozirconium precatalyst and borate cocatalyst produce the desired polyethylenes with excellent activity and branch selectivity.
Establishing an efficient catalytic system for direct amidation reactions has remained a formidable challenge for years. This Comment will focus on potential new directions in the hope of moving this field forward.