Browse Articles

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.

Incorporating main group elements into amorphous porous organic polymers has enabled the fine tuning of the structures and properties of these materials. Here, the authors review studies in which the geometric structures and electronic properties of main group elements have influenced material structures and properties, and whereby their incorporation has enabled new strategies to synthesize such materials.

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.

Artificial photosynthesis aims to produce fuels and chemicals from simple, abundant building blocks, such as water and carbon dioxide, with sunlight as a source of energy. Here, the authors review recent developments in biomimetic, compartmentalized vesicular systems towards artificial photosynthesis, and highlight challenges and opportunities in mimicking this complex natural reaction system.

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.

Shortwave UV photons and very low energy electrons (vLEEs) are thought to be unfavorable prebiotic conditions on early Earth which can destroy unstable molecules. Here, the authors propose that nucleobases in their complementary pairs can enhance and consolidate the intrinsic stability of nucleobases against shortwave UV photons and vLEEs and promote their proliferation.

Seleno-insulins (SeIns) are known to exhibit different in vitro properties from wild-type insulin, upon replacement of one of the three disulfide bonds with diselenide bonds; however, the in vivo hypoglycemic effect remains poorly understood. Here, the authors optimize the synthesis of SeIns via native chain assembly and reveal in vitro resistance against the insulin-degrading enzyme, as well as the in vivo hypoglycemic effect in diabetic rats at a dose of 150 μg/300 g rat.

Late-stage functionalization of drug molecules can tune their properties without the need for entirely new syntheses, however, predicting reactivity and planning synthesis for late-stage C-H activation remains challenging. Here, the authors develop a reaction screening approach combining high-throughput experimentation with computational graph neural networks to identify suitable substrates that can be used for late-stage C-H alkylation via Minisci-type chemistry.

β-Amino acid-containing macrolactams are a known natural product family exhibiting structural and functional diversity, however, the natural chemical space of this family remains underexplored. Here, the authors use a targeted β-amino acid-specific homology-based multi-query search to identify their potential microbial producers, explore the variation of their biosynthetic gene clusters, heterologously produce ciromicin A, and identify new macrotermycin derivatives.

The reduction of dinitrogen to ammonia catalyzed by nitrogenase involves long-range conformational changes within the enzyme complex, however, direct biophysical evidence of communication between the Fe protein and the MoFe protein is lacking. Here, the authors combine millisecond time-resolved hydrogen-deuterium exchange mass spectrometry and normal mode analysis, revealing molecular-level insights into how the Fe protein alters the stability and dynamics of the MoFe protein near the active site in a nucleotide-dependent manner.

Tetraphenylethylenes (TPEs) are known for their aggregation-induced emission and electrochemical properties of value for optical sensors, however, established synthetic routes suffer from several limitations. Here, the authors develop a metal-free route to TPEs and other alkenes via a sulfur-mediated coupling of N-tosylhydrazones, achieving good yields and a broad substrate scope.