Research articles

Ultra-high molecular weight (UHMW) polymers exhibit exceptional mechanical properties and have found extensive applications, however, it remains challenging to produce them with a low dispersity. Here, the authors develop ultrasound-initiated copolymerization of diverse monomers, generating UHMW polymers with low dispersity within 15 min.

Solution NMR spectroscopy provides rich structural information on biomolecules, however, its resolution becomes limited when molecular size increases, due to short-lived nuclear magnetic responses to electromagnetic radiation. Here, the authors sustain long-lived coherences for the aliphatic protons of glycine residues within protein lysozyme, yielding substantial through-space magnetization transfers, and mapping interacting atoms in the protein structure.

Plasma-activated chemical transformations promise efficient syntheses of vital chemicals such as ammonia, however, reaction pathways are often unknown and quantum state-resolved information is lacking. Here, the authors use quantum cascade laser dual-comb spectroscopy to study non-thermal plasma-activated ammonia synthesis with rotational and vibrational state resolution, quantifying state-specific number densities via broadband spectral analysis.

Tandem mass spectrometry spectra contain structural information of analyzed small molecules, however structural annotation and prediction from MS spectra remain challenging. Here, the authors combine the fragmentation tree models with a deep-learning transformer module, to annotate the fragmentation peaks and generate de novo molecular structures from a low-resolution mass spectrometer.

The anthraquinone process is currently the predominant method for large-scale H₂O₂ production, but the reaction’s high energy consumption and hazardous waste generation spur the search for alternatives. Here, the authors investigate the two-electron oxygen reduction reactivities of metal-free non-porous, micro-, and mesoporous carbon catalysts to elucidate the impacts of porous structures, finding mesoporous structures show the highest H₂O₂ production selectivity.

Graphene quantum dots have versatile properties, but their luminescence can be quenched when the dots aggregate. Here, the authors immobilize graphene quantum dots on 2D MOF sheets and demonstrate their photoluminescence in suspension and as a dry powder, and show their application in copper ion sensing.

Thiolate groups are promising anchors to immobilize catalysts, particularly on coinage metal surfaces, but the anchor group’s impact on the local adsorption configuration of the catalyst is often overlooked. Here, the authors study a sulfurated derivative of the prominent Re(bpy)(CO)3Cl carbon dioxide reduction catalysts on a Ag(001) surface at room temperature.

Ligand-based reverse screening plays an important role in predicting molecular targets of bioactive compounds, however, its predictive ability might be overlooked due to the limitations of existing external test sets. Here, the authors assess the predictive power of reverse screening with a large diverse external bioactivity dataset.

The strong electric field between the tip of a scanning tunneling microscope and graphite has been used to modulate the two-dimensional polymerization of aryl boronic acids. Here, the authors study the influence of solvent choice and monomer concentration on the electric field-mediated polymerization and depolymerization of a boroxine-based 2D polymer on graphite.

Establishing biotechnological alternatives to chemical syntheses requires the rational design of biosynthetic pathways and degradation routes either as enzymatic cascades in vitro or as part of living organisms. Here, the authors use alanine dehydrogenase from Vibrio proteolyticus and the diaminopimelate dehydrogenase from Symbiobacterium thermophilum for the in vitro production of (R) and (S)-3-fluoroalanine, reaching >85% yield with complete enantiomeric excess.

Identifying the short-lived intermediates and reaction mechanisms of multichannel radical cation fragmentation processes remains a current and important challenge to understanding and predicting mass spectra. Here, the authors show that coherent oscillations in the femtosecond time-dependent yields of several product ions following ultrafast strong-field ionization of endo-dicyclopentadiene represent spectroscopic signatures that elucidate their mechanism of formation and identify the intermediate(s) they originate from.

Breakthroughs in the efficient use of biogas fuel depend on the successful separation of carbon dioxide/methane streams and identification of appropriate separation materials. Here, machine learning models are trained to predict biogas separation properties of metal-organic frameworks.

Label-free detection of nucleic acids such as microRNAs holds great potential for early diagnostics of various types of cancers, but insufficient detection limits hamper applicability. Here, the authors use nitrogen-vacancy centers in diamond to measure the intrinsic magnetic noise of paramagnetic counter ions interacting with microRNAs, lowering the detection limit to ~23 miR-21s.

Targeting RNA with small molecules represents an attractive medicinal approach, and profiling the small molecule-binding landscapes of various types of RNA structures is critical. Here, the authors develop a large-scale approach for investigating small molecule-RNA structure interaction profiles using a multiplexed pull-down assay with various RNA structure libraries, and validate the assay using G-clamp and thiazole orange derivatives.

Biomolecular coacervates are emerging model systems to understand biological processes. Here, the authors reveal details on how the length and sequence of the DNA binders influence the multivalency-driven coacervate formation, how to introduce switching and autonomous behavior in reaction circuits, as well as how to engineer wetting, engulfment, and fusion in multi-coacervate system.

Aldo-keto reductase 1C3 (AKR1C3) is known to be a cancer biomarker correlated to androgen synthesis, and causes drug resistance by direct action on chemotherapeutics and by stabilizing AR splice variant 7 (ARv7). While selective inhibitors against AKR1C3 are developed, the ARv7 is thought to be undruggable. Here, the authors develop an AKR1C3-ARv7 dual PROTAC degrader based on a selective inhibitor against AKR1C3, showing the potential for degradation of AKR1C3 and ARv7 simultaneously.

The fluorine isotope ¹⁸F is a PET nuclide used for imaging studies, but the incorporation of [¹⁸F]HF into 2,2-difluorovinyl groups to generate radiotracers and labeling reagents has only been achieved in low yields. Here, using a combination of Et₃SiH and TEMPO in the absence of oxidizing agents is shown to afford a higher yield, better product quality, and controllable selectivity between the formation of a S–F or C–F bond.

Amides are important intermediates in organic chemistry and the pharmaceutical industry, but their low reactivity requires catalysts and/or harsh reaction conditions to esterify them. Here, the authors report a versatile and mild dimethyl sulfate-mediated reaction to activate and esterify C—N bonds, achieving up to 95% amide bond cleavage.

Organosodium compounds are appealing sustainable alternatives to precious transition metal compounds, yet they have rarely been used in homogeneous catalysis. Here, the authors introduce a dihydropyridylsodium compound, Na1,2-tBu-DH(DMAP), and its monomeric variant [Na-1,2-tBuDH(DMAP)]·Me₆TREN, and demonstrate their effectiveness in transfer hydrogenation catalysis of a representative alkene, 1,1-diphenylethylene, using 1,4-cyclohexadiene as a hydrogen source.

Peptide condensates are known to regulate compartmentalized enzymatic reactions, however, the influence of condensate chemical composition on enzymatic reactions is still poorly understood. Here, the authors study β-galactosidase as a simple enzymatic model and reveal that product formation is enhanced in heterotypic peptide-RNA condensates, but the reaction is restricted in homotypic peptide condensates.