Research articles

Conversion of methane to methanol via methanol derivatives such as methyl bisulfate (MBS) allows to achieve high selectivity and yield, but separating MBS from oxidizing agents such as sulfuric acid is an energy-intense step. Here, the authors eliminate the need for separation of MBS from sulfuric acid by replacing the former with methyl trifluoroacetate, which is subsequently hydrolyzed into high-purity methanol.

Metal–organic frameworks functionalized with photoresponsive molecules are of interest as materials with photoswitchable electronic properties, but designing such MOFs remains challenging. Here, the authors use in silico molecular design to explore photoswitchable MOF candidates that incorporate spiropyran photoswitches at controlled positions and with defined intermolecular distances and orientations.

Understanding the atomic dynamics of active catalyst sites is crucial for the precise optimization of catalyst performance. Here, the authors employ operando XAFS and DRIFTS to study the dynamics of the mobility of platinum and copper dopants in bimetallic and trimetallic gold nanoclusters supported on ceria, using the water-gas shift process as a model reaction.

Angucyclines are a class of natural products that harbor unusual structural rearrangements through B- or C-ring cleavage of their tetracyclic backbone, however, the enzymes leading to C-ring cleavage remain poorly understood. Here, the authors use targeted gene deletion and complementation as well as metabolomics to study the function of putative oxygenases involved in lugdunomycin biosynthesis, and reveal their potential roles towards C-ring cleavage.

The water surface has recently proven to be an effective platform for the synthesis of large-area two-dimensional polymers with high crystallinity. Here, the authors report the on-water synthesis of a crystalline monolayer 2D polyimide, as well as its incorporation into organic–inorganic hybrid van der Waals heterostructures that display significant charge transfer and high electron mobility.

Nucleophilic addition reactions of propargyl cations can result in diverse synthetically useful compounds, however, dehydrative propargylation through α-alkyl-propargyl cations remains challenging. Here, the authors utilize a highly oxophilic indium cation to generate α-alkyl-propargyl cations from secondary alcohols and apply them to S_N1-propargylation.

Human interleukin-10 (IL-10) is known to be an immunosuppressive cytokine for anti-inflammation, however, IL-10 can enable the evasion of tumor cells through immunosuppression of the host immune system. Here, the authors develop an IL-10 inhibitory peptide, NK20a, that displays anticancer effects, and show that its conjugation with chemotherapeutic gold nanoparticles enhances their anticancer efficacy.

Feedstock properties play a crucial role in thermal conversion processes for power generation, fuel production, or chemical synthesis, but understanding the influence of these many properties on treatment performance is a complex task. Here, a series of van Krevelen diagrams were generated to illustrate the impact of H/C and O/C ratios of feedstock on the products obtained from six commonly used thermochemical processes.

Protein hydration shells play an important role in protein function, however, regulation of the hydration shell remains underexplored. Here, the authors use small-angle scattering (SAS) data in solution as a protein-specific probe, quantitatively compare SAS data with explicit-solvent SAS prediction by molecular simulations, and reveal the effect of protein charge and geometric shape on the hydration shell.

Single atom catalysts dispersed on a surface demonstrate great promise for a variety of catalytic reactions, but their aggregation leads to a degradation of catalytic activity. Here, the authors use quantum mechanical calculations to study the catalytic activity of Cu adatoms stabilized with N-heterocyclic carbenes (NHCs) on a Cu(100) surface, finding that NHC-decoration significantly reduces the energy barriers to electrocatalytic CO hydrogenation and C–C coupling.

Compression is a common densification method for solid-state materials, but the structural evolution of compressed non-equilibrium oxide materials such as glasses and zeolites remains somewhat elusive. Here, the authors show that siliceous zeolite single-crystals cold-compressed at 20 GPa yield permanently densified glassy silica, while cold-compressed siliceous zeolite powder and glassy silica are metastable.

The on-surface synthesis of graphene nanoribbons with control over their length and final surface coverage is desirable for electronic applications. Here, the authors outline a protocol to produce long and isolated graphene nanoribbons on an Au(111) surface, achieving lengths of up coverage down to ~0.4 monolayer, of potential value for mono-molecular electronics. to 50 nm and a low surface coverage down to ~0.4 monolayer, of potential value for mono-molecular electronics.

The abiotic production of molecular oxygen in carbon dioxide-rich planetary atmospheres is important in understanding astrochemical reactions and potentially the origin of life on Earth. Here, the authors demonstrate that the low-energy reaction between helium ions, as found in solar winds, and carbon dioxide produces molecular oxygen.

The electrolytic reduction of CO₂ in aqueous media promises a pathway for the utilization of the greenhouse gas by converting it to base chemicals, however, reactions at the electrodes and their proximity remain challenging to elucidate. Here, the authors use multinuclear in operando NMR to study CO₂ electrolysis in aqueous media and find that stable ion pairs in solution catalyze the bicarbonate dehydration reaction.

Diterpene glycosyltransferase UGT76G1 is a key enzyme in the biosynthesis of rebaudioside A, a naturally sweet-tasting compound, however, its poor thermostability hinders its industrial application. Here, the authors use a computational design strategy to generate a mutant of UGT76G1 that exhibits improved thermostability and enzymatic activity.

Platinum dispersed on metal oxide supports is widely used for industrially important catalysis such as the reverse water gas shift reaction, but active site migration and subsequent alterations in catalytic performance are still not fully understood. Here, the use of platinum on ceria nanodomes shows the detrimental effect of migration of platinum nanoparticles to titania supports at elevated temperatures.

Gas chromatography is a useful tool to identify and characterize wines, usually by selecting some compounds for a particular classification problem, yet, with limited success. Here, the authors decode the estates perfectly and age 50% correctly of twelve red Bordeaux wines from unrestricted, raw gas chromatograms using machine learning.

Non-cell-permeable cryoprotectants exhibit cryopreserving effects by preventing intracellular ice crystal formation, but these can damage cells due to high osmotic pressure and dehydration. Here, the authors developed a poly(zwitterion) isotonic cryoprotectant that forms a firm matrix around cells that prevents the influx of ice crystal nuclei without the need for high osmotic pressure and dehydration.

Atom-centered neural networks represent the state-of-the-art for approximating quantum chemical properties of molecules, such as internal energies, but the final atom pooling operation that is necessary to convert from atomic to molecular representations in most models remains relatively undeveloped. Here, the authors report a learnable pooling operation, usable as a drop-in replacement, that leverages an attention mechanism to model interactions between atom representations.

The variable frequency microwave (VFM) technology is known for its theoretically uniform microwave E-field distribution, although the experimental distribution remains poorly understood. Here, the authors examine the effectiveness of VFM irradiation experimentally by in situ 3D observation of the E-field, and apply VFM to the large scale synthesis of 4-methylbiphenyl via the Suzuki-Miyaura cross-coupling reaction catalyzed by solid Pd supported on activated carbon particulates.