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Molecularly well-defined single-site catalysts are very promising from an atom utilization perspective, as well as for a potential fine-tuning of the single-site environment. Now, high water oxidation performance is reported on a π-conjugated microporous polymer with single Co sites, which follows an intramolecular hydroxyl nucleophilic attack that promotes O–O formation.
The electrochemical generation of reactive hydrides has the potential to drive the electrification of chemical reactions. Now, a modified electron paramagnetic resonance set-up is put forward to demonstrate the role of Mo3+ hydride in amorphous MoSx to catalyse both the hydrogen evolution reaction and electrochemical NADH regeneration.
The use of ammonia as a nitrogen source in catalytic asymmetric reactions is attractive but represents a difficult exercise. Now, the asymmetric synthesis of N-unprotected α-amino esters from α-diazoesters and ammonia is achieved by cooperative action of copper complexes and chiral hydrogen-bond donors.
A recently proposed structure of an N2-bound Mo-nitrogenase has sparked considerable attention, although the direct evidence for N2 binding and sulfur mobilization during turnover has remained elusive. Now, additional spectroscopic and kinetic measurements further support this state and provide evidence that belt-sulfur displacement is an essential aspect of the nitrogenase mechanism.
Engineering enzymes to perform new-to-nature reactions can address long-standing challenges in synthetic chemistry. Now a ketoreductase has been evolved to undergo a photoinduced single-electron-transfer pathway, thereby achieving an enantioselective Giese-type radical conjugate addition that yields α-chiral esters.
Integrated electro-biocatalytic systems based on immobilization have been limited by low maximum current density. Here, the authors present spatially separated electrocatalytic CO2 fixation to acetic acid with high activity, as feedstock for fermentation by genetically engineered yeast to produce complex bioproducts including glucose and fatty acids.
Bases play a fundamental role in several iconic coupling reactions in organic chemistry but are simultaneously responsible for limitations, such as functional group tolerance. Now, a broadly applicable solution is presented that uses non-innocent electrophiles equipped with an encrypted base.
High-performance approaches for terpenoid discovery and characterization in fungi are lacking. Now, a fully automated and high-throughput biofoundry is developed using Aspergillus oryzae as chassis for efficient genome mining and biosynthetic pathway analysis of bioactive terpenoids.
Single-atom catalysts consisting of isolated iron sites on a nitrogen-doped carbon matrix (Fe–N–C) are very promising cathode catalysts for proton exchange membrane fuel cells (PEMFC), but it is challenging to achieve a high density of single iron sites. Now, a synthetic approach is introduced to afford high-density Fe–N–C catalysts with a high PEMFC performance.
The relationship between product selectivity and catalyst structure under dynamic reaction conditions has proved difficult to interpret in electrocatalytic CO2 reduction. Here, the authors combine operando X-ray techniques with high time resolution to investigate control over product selectivity using potential pulses.
Structure sensitivity is an important property in catalysis, although its determination at the atomic cluster scale remains difficult. Here, the authors explore the reactivity of different palladium clusters with low nuclearity identifying the ideal Pd–Pd coordination number for the dehydrogenation of dodecahydro-N-ethylcarbazole.
Ground state destabilization is often evoked as a possible explanation of orotidine-5′-phosphate decarboxylase catalysis. Now, high-resolution structures of this enzyme provide time-resolved snapshots along its reaction coordinate revealing that transition-state stabilization by electrostatic interactions drives its reactivity.
Atom trapping is a well-established route to prepare single-atom catalysts. Here the authors propose a reverse atom-trapping strategy in which surface strontium atoms of LSCF fuel cell cathodes are extracted by MoO3, forming single strontium vacancies on LSCF in a controllable manner and tuning its performance for the oxygen reduction reaction.
Crossover of CO2, in the form of carbonate, from the cathode to the anodic compartment places a major limitation on carbon efficiency in traditional CO2 electrolysis cells. Here, the authors place a porous solid electrolyte layer between the compartments, where protonation of carbonate during CO2 electrolysis allows recovery of over 90% of the lost CO2 gas.
Acidic media provide an opportunity to alleviate carbonate formation in electrocatalytic CO2 reduction but increase competition from H2 evolution. This study demonstrates that alkali cations in acidic media suppress H2 evolution leading to high Faradaic efficiency for carbon-based products and models the physical effects that lead to this result.
Electrocatalytic CO reduction presents a route to low-temperature acetate production, but activity and efficiency remain below practical levels. Here, the authors present an intermetallic compound with stable, atomically ordered Cu–Pd pairs that facilitates an acetate pathway and delivers 70% Faradaic efficiency at 425 mA cm−2.
PtRu nanoparticles are the state-of-the-art catalysts for methanol electrooxidation—the anodic reaction in direct methanol fuel cells. Now, a method of dispersing single Pt atoms over Ru nanoparticles is presented and monitored in situ, thereby boosting the catalytic performance in the methanol oxidation reaction.
Ammonia is industrially synthesized through an established process based on iron or ruthenium transition metal catalysts, although the quest for alternative and more sustainable processes is still ongoing. Here, the authors show that potassium hydride confined between graphene layers can reduce dinitrogen and catalyse ammonia synthesis under mild conditions.
The scarcity and high price of noble metal catalysts pose critical challenges for the chemical industry, and finding strategies that ensure complete atom efficiency has become a pivotal endeavour. This work introduces the fabrication of amorphous single-layer PtSex catalysts for the hydrogen evolution reaction with high atom-utilization efficiency.
Poor management of gas flow limits efficiency in tandem (two-catalyst) electrocatalytic CO2 reduction. Here, the authors develop a segmented gas-diffusion electrode architecture that prolongs the residence time of CO (produced by the first catalyst) at the second catalyst, resulting in high production of further reduced yields.