Research articles

Computational methods enable the rapid evaluation of the gas uptake capabilities of metal–organic frameworks. Here, MOFs are screened for their CO₂ capture abilities using machine learning trained on molecular simulation data, with new effective point charge descriptors introduced to aid this process.

Electrochemical reduction of carbonyl groups is a promising sustainable route for converting biomass-based compounds into value-added products. Here, the authors investigate the electrochemical reduction of the model reactants formaldehyde, acetaldehyde, and acetone on single-site M–N–C catalysts (M = Fe, Co and Ni), gaining mechanistic insight into the role that the nature of the metal center plays on the selectivity of these carbonyl reduction reactions.

Supersaturated amorphous drug–salt–polymer systems are known to improve the aqueous solubility of poorly water-soluble drugs as well as their bioavailability, however, the rational optimization of such systems is largely unexplored. Here, the authors optimize the polymer and salt combination for the drug celecoxib and achieve improved biopharmaceutical performance by experimental and computational characterization of their amorphous solid dispersions.

D-Amino acids are widely present in nature and display diverse physiological functions, however, their large-scale synthesis remains challenging for specific amino acids. Here, the authors design hyper-thermostable ancestral L-amino acid oxidases (HTAncLAAO2), catalyzing the chemoenzymatic synthesis of D-tryptophan from L-tryptophan at a preparative scale.

The simultaneous electroreduction of carbon dioxide and nitrate is a promising and environmentally benign route to urea production, but achieving high selectivity for urea electrosynthesis via this route remains challenging. Here, CuO_xZnO_y electrodes are shown to enable the efficient and selective production of urea under mild conditions, with the efficiency found to strongly depend on the metal ratio within the catalyst composition.

Heterogeneous reaction of NO₂ with atmospheric humic like substances is a potentially important source of volatile organic compounds, but the role of ubiquitous water-soluble aerosol components in this chemistry remains largely unexplored. Here, secondary electrospray ionization ultrahigh-resolution mass spectrometry is used to obtain real-time measurements of VOCs formed during the heterogeneous reaction of gas phase NO₂ and a solution containing gallic acid as a model for moderately acidic aerosol particles.

Fluorinated ketones can function as covalent warheads applied in the design of reversible covalent inhibitors, however, the reactivity of certain fluorinated moieties remains underexplored. Here, the authors investigate the species-specific lipophilicities of fluorinated geminal diketones in multicomponent equilibrium systems and reveal their potential as multifaceted warheads for reversible covalent drugs.

Co-electrolysis of nitrogen oxides and carbon oxides has been studied for over two decades but remains largely inefficient with numerous persisting knowledge voids. Here, the authors report a thermodynamic basis for modelling urea production via co-electrolysis using several exchange-correlation functionals, highlighting the importance of gas-phase error assessment in computational electrocatalysis.

One-carbon insertion into N–O bonds is widely exploited in organic synthesis, but synthetic protocols for this rely on hazardous diazo precursors that are difficult to access. Here, copper-catalyzed intermolecular formal (5 + 1) annulation of 1,5-diynes with 1,2,5-oxadiazoles is shown to facilitate one-carbon insertion into heterocyclic N–O bonds without the need for diazo precursors.

Electrolytes with high concentrations are desirable for high-performance electrochemical devices, but their microstructures are still not well understood. Here, the authors study electrolyte structure and correlate it to ionic conductivity for four nitrate-based electrolyte solutions over wide concentration and temperature ranges, and derive a simple model with only two parameters and high accuracy to correlate conductivity with molar concentration and temperature.

Microbial enzymes are capable of degrading certain synthetic polymers, with most polyethylene terephthalate (PET) degrading enzymes known to derive from bacteria or fungi. Here, the authors describe an archaeal originating feruloyl-esterase PET46 enzyme with a flexible lid domain and PET degradation capability.

Proteins that are able to switch between different folds correlate their structural and functional changes, however, crowding effects on fold-switching proteins are not fully understood. Here, the authors study the fold switch of the protein G domains G_A and G_B using a structure-based dual-basin model, revealing a crowding-induced G_A-to-G_B fold switch, and elucidating the role of a disordered range in G_A.

Iron–sulfur clusters are important cofactors involved in a wide range of protein functions, however, the incorporation of FeS clusters into proteins remains underexplored. Here, the authors report the crystal structure of a Zn-containing form of a Rieske protein, in which ZnCl₂ binds in an FeS-binding site, representing a putative immature form of a Rieske protein prior to FeS insertion.

Monitoring glycosylation is a key quality control for protein therapeutics, however, most established methods such as hydrophilic interaction chromatography with fluorescence detection (HILIC-Fld) and liquid chromatography-mass spectrometry (LC-MS) require time-consuming procedures and complicated data analysis. Here, the authors apply high performance anion exchange chromatography coupled to pulsed amperometric detection (HPAEC-PAD) for the batch-to-batch monitoring of glycans on complex antigens with a simplified procedure.

AlphaFold2 is a popular protein structure prediction tool, however, achieving high accuracy remains challenging for certain proteins that share fewer homologs with the database. Here, the authors develop a new version of the MULTICOM system to improve the multi-sequence alignment, structural template, model ranking, model refinement, and hence the accuracy of AlphaFold2 prediction.

Spirosorbicillinols A–C are fungal natural products that display various biological properties, but their total synthesis has yet to be accomplished. Here, the authors report the total synthesis of spirosorbicillinols A–C based on a chemo-enzymatic transformation of sorbicillin into sorbicillinol, which is fused to synthetically prepared scytolide and isomers by a Diels-Alder cycloaddition reaction.

Amyotrophic lateral sclerosis (ALS) is associated with the misfolding of hSOD1 and C71G-hPFN1, however, the exact mechanism responsible for ALS remains poorly understood. Here, NMR spectroscopy reveals that ATP can induce the folding of hSOD1 and C71G-hPFN1, inhibiting protein aggregation and enhancing their thermodynamic stability.

Understanding the mechanical properties of metal–organic frameworks (MOFs) is crucial for their industrial application, but the compressibility of structurally dynamic MOFs under pressure remains unclear. Here, in situ variable pressure powder X-ray diffraction experiments on two families of dynamic MOFs find that increased structural flexibility results in enhanced mechanical resilience.

The inhibition of cytochrome P450 (CYP) enzymes is central to many therapeutics, however, achieving selectivity across CYP enzymes remains challenging. Here, the authors develop isonitrile-harboring steroids as selective steroidogenic CYP heme iron ligands.

Cross-dehydrogenative coupling is an efficient route for C–C bond formation by direct C–H functionalization, however, this protocol usually requires stoichiometric oxidants under harsh reaction conditions. Here, the authors report a cross-dehydrogenative Minisci-alkylation using a heterogeneous Rh₂O₃/GaN photocatalyst and a benzophenone photosensitizer under oxidant-free conditions.