Articles in 2023

The sluggish conversion of lithium polysulfides in Li–S batteries can be overcome by the use of catalysts, but their design is typically done via trial and error. Now, a binary descriptor is proposed by machine learning to capture electronic and structural effects for the design of Li–S battery cathode catalysts.

CO₂ electroreduction is a promising process for the production of high-value chemicals, but achieving high selectivities for specific products is challenging. Now, a Faradaic efficiency of 87% for acetate is achieved on a Cu/CuO_x catalyst under 58 atm CO₂(g), where high and low concentrations of dissolved CO₂(aq) and proton donor HCO₃⁻ are shown to promote acetate formation, respectively.

Understanding the structure–performance relationships of heterogeneous catalysts is of fundamental importance for their deployment in industry. However, gaps exist between the conditions and catalytic materials commonly employed in laboratory studies and those encountered in practical reactors. This Perspective highlights the importance of recognizing such gaps, with the goal to inform the planning of academic research and maximize its impact.

Plasmonic photocatalysis presents opportunities for efficient utilization of sunlight for chemical transformations, yet its mechanisms, including the relative contribution of thermal and non-thermal effects, remain controversial. Here the authors develop methodology to monitor both effects and propose a metric, overall light effectiveness, to evaluate and maximize the total light-driven enhancement.

Controlling strong metal–support interactions to promote catalytic performance is a desirable yet challenging endeavour. Now, the in situ formation of TiO_x patches on an MnO support, instead of encapsulated metal, facilitates hydrogen spillover and promotes the reverse water-gas shift reaction performance.

Enantioselective C–C cross-coupling of unactivated alkenes is challenging. Now, nickel catalysts bearing bulky C₂-symmetric chiral N-heterocyclic carbene ligands enable directing group-free asymmetric cross-coupling of unactivated alkenes with aryl or alkenyl triflates and nucleophiles, generating C sp³ stereocentres.

Cas9 is a powerful genome-manipulation enzyme, although how its catalytic activity is controlled is not completely solved. Now, cryo-electron microscopy structures of Acidothermus cellulolyticus Cas9 provide atomic-level insights into its activation involving DNA binding, conformational changes and the formation of its two active sites.

Alkene 1,1-difunctionalization can provide direct access to valuable molecules. Now, an organometallic-radical relay strategy involving radical generation through homolysis of the metal–alkyl complex allows catalytic coupling of terminal or internal alkenes with arylboronic acids and electrophilic radical acceptors.

The selective hydrogenation of acetylene to ethylene involves high H₂ consumption as well as a high energy input. Now, a thermocatalytic process for acetylene semi-hydrogenation using H₂O as H source and CO on a Au/α-MoC catalyst is introduced.

CO electroreduction is a promising process for obtaining high-value chemicals but it typically suffers from low durability. Now the degradation mechanisms of membrane-electrode-assembly devices during high-rate CO reduction are identified via operando wide-angle X-ray scattering measurements and circumvented.

Inexpensive Fe–N–C single-atom catalysts are a promising solution to replace costly Pt-based cathode catalysts in fuel cells, but they typically suffer from low durability. Now, the degradation mechanisms of Fe–N–C catalysts are identified under operando conditions as a function of time, and potential solutions are proposed.

The electrochemical conversion of carbon dioxide to high-value multicarbon products is very desirable, but also fraught with immense complexity in process design. A twist in tuning product yields in this reaction could be based on water activity.

The electrochemical reduction of CO₂ in strong acids is difficult. Now a strategy utilizing immobilized cations significantly enhances system stability and efficiency, opening up avenues for optimized CO₂ conversion to C₂ products.

Upgrading methane to more valuable chemicals such as methanol is highly appealing but remains challenging. Here the authors show how edge-rich MoS₂ can be used to oxidize methane to C1 oxygenates at room temperature using oxygen as the oxidant.

The valorization of methane into oxygenated products has long intrigued the catalysis community, however, progress in the field is disparate and practical implementation remains elusive. This Review discusses recent advances in the area using performance indicators that reveal the gaps between academic investigations and industrial methane utilization and highlight possibilities for further developments.

CO₂ conversion to valuable chemicals is of great interest in sustainable chemistry. Now, β-amino acids are synthesized by a dual catalytic strategy that enables the aminocarboxylation of alkenes using CO₂, proceeding via alkene radical anion intermediates that are generated using a designed binaphthol-derived photoredox catalyst.

The electrochemical synthesis of hydrazine is a very attractive yet challenging process. Now, the direct electrochemical oxidation of ammonia to hydrazine on a Ru complex catalyst, involving a bimolecular N‒N coupling mechanism, is reported.