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The ab initio atomistic thermodynamics approach, coined by Reuter and Scheffler formally in 2001, remains pivotal for understanding and predicting the stable surfaces of thermal catalysts under technical conditions.
Traditional catalyst synthesis primarily hinges on liquid-phase methods. Nevertheless, a quarter of a century ago, the advent of vapour-phase methods such as atomic layer deposition opened up important alternatives to atomically tailor catalysts and boost their performance.
Electrocatalysis would not be the same without the rotating disk electrode. Its invention in the mid-twentieth century enabled immense developments, which rendered it a classic technique in electrochemistry. The rotating disk electrode will remain a cornerstone of electrocatalysis with further advances that bridge the gap with real systems.
Acetyl-CoA carboxylation is the canonical route for endogenous malonyl-CoA formation in cells. Here, the authors design a non-carboxylative malonyl-CoA pathway independent of acetyl-CoA into multiple microbes for efficient malonyl-CoA-derived natural products biosynthesis.
The mechanism by which bimetallic catalysts can outperform their monometallic counterparts is often unexplained. Now nitrate hydrogenation on bimetallic catalysts is shown to proceed via the electrochemical coupling of hydrogen oxidation and nitrate reduction half-reactions, each of which occurs on one metal component.
Axial chirality is a key element in many valuable compounds, such as ligands in organic chemistry or pharmaceuticals. Now the catalytic atroposelective synthesis of acyclic 1,3-dienes by chiral phosphoric acid-catalysed bromination is described, expanding the chemical space of axially chiral compounds.
Precious-metal-free catalysts for water oxidation commonly suffer from low stability in acidic electrolytes. Now, by controlling the intergrowth of the γ-MnO2 structure, it has been possible to achieve 2 A cm−2 at 2 V and a stability of over 1,000 hours at 200 mA cm−2 in a polymer electrolyte membrane electrolyser.
The generation of Fischer-type carbene complexes for organic synthesis usually requires stoichiometric amounts of metal. Now the palladium-catalysed formation of a Fischer-type carbene intermediate for the synthesis of β-lactam derivatives is described and its crystal structure is solved.
Single metal atom catalysts on N-doped carbon supports are promising materials to replace Pt as cathode catalysts in fuel cells. Now a transient voltammetry method is applied to extract the kinetic and thermodynamic parameters of the oxygen reduction reaction on an iron phthalocyanine model catalyst.
Fixing CO2 into value-added solid carbon such as carbon nanofibres is a promising process but poses substantial challenges. Now a tandem strategy is proposed where CO2 and water are electrocatalytically converted into syngas to subsequently form carbon nanofibres via a thermocatalytic process.
Ring-expanding carbon-atom insertion reactions are currently limited to the installation of few functional groups. Now researchers show the use of a radical carbyne precursor for the insertion of carbon atoms bearing varied functional groups to access 2-substituted naphthalenes from indene.
Heterogeneous catalysts are often dynamic under operation. Now, the mechanism of CH4 dry reforming on Ni is studied by in situ microscopy and spectroscopy, revealing the formation of metastable surface nickel–oxygen structures from CO2 dissociation that exhibit different catalytic properties and induce rate oscillations.
The electrochemical deoxygenation of carbonyl groups by hydrogenolysis is challenging as the competing hydrogenation usually prevails. Now the electrochemical Clemmensen reduction is proposed, achieving the selective hydrogenolysis of various carbonyl compounds using Zn as the electrocatalyst in a mildly acidic solution.
Photocatalytic overall water splitting on particulate systems represents a possibility for clean energy storage, yet efficiencies for the process are typically low. Here, highly concentrated saltwater is used to polarize photoexcited N-doped TiO2, resulting in enhanced charge separation and a solar-to-hydrogen efficiency approaching 20%.
Coenzyme Q has several important biological functions, but the understanding of the biosynthesis of coenzyme Q in humans remains incomplete. Now, by constructing the entire COQ metabolon in vitro, the enzymes and reactions underlying coenzyme Q biosynthesis are characterized.
The reconstruction of Cu electrocatalysts during CO2 reduction is an impediment to the stability of this technology, yet a clear picture of the species involved in this process remains elusive. Here, the authors demonstrate the presence of transient solution-based Cu(I) species and theoretically predict complexes with CO and oxalate as the likely candidates.
C–C bond formation involving sp3 centres has typically relied on stoichiometric reagents. Here catalytic Ag electrodes modified with Mg(OAc)2 enable electrocatalytic coupling of an organic halide with an aldehyde for the selective formation of a broad scope of alcohol products.
Using N2 as a N source to nitrogenate compounds is highly desirable but also very challenging. Now a cascade electrosynthesis strategy is proposed to prepare (CF3SO2)2NLi and its analogues from N2 via a looped Li–N2 battery.