Articles in 2022

3,3,3-Trifluoropropene is a cost-efficient precursor for the preparation of trifluoromethylated compounds, but limited methods for its efficient transformation have been reported. Here, nickel-catalyzed alkyl-arylation of 3,3,3-trifluoropropene with tertiary alkyl iodides and arylzinc reagents is achieved with high efficiency.

Training datasets for artificial intelligence based chemistry models typically rely on experimental data from optimised synthetic conditions only, leading to an inherited bias in the model predictions. Here, the authors develop an artificial intelligence model based on a variational autoencoder to synthetically generate continuous datasets and generate new chemical reactions in a less biased way, by sampling the entirety of the solution space.

Atomically precise control of the structure and coordination of protein-protected Au nanoclusters remains a challenge. Here, the authors synthesize and characterize a multinuclear Au nanocluster using a 4-fold symmetric axis channel of an apo-ferritin cage as a scaffold, and identify key protein residues during the Au accumulation process.

Amine mixtures are industrially used for carbon capture, whereby sluggish reaction kinetics are sped up with piperazine additives. Here, the authors report an experimentally verified computational approach that combines kinetic experiments, molecular simulations, and machine learning to identify a class of tertiary amines that absorbs CO₂ faster than a typical commercial solvent when mixed with piperazine.

Molecular dynamics simulations, used to study chemical and biophysical processes, rely on the accuracy of the employed force fields. Here, the authors review successes and key areas of difficulty in the development of additive and polarizable force fields, and discuss experimental data availability, how empirical refinement impacts parametrization, and highlight possible routes to further improve the accuracy of force fields.

Fibroblast growth factor receptor 4 (FGFR4) is a promising target for the treatment of hepatocellular carcinoma, but current FGFR4 covalent inhibitors target only one of the two cysteine residues (Cys477 or Cys552) that provide FGFR4-specificity. Here, a dual-warhead covalent FGFR4 inhibitor that can covalently target both cysteine residues of FGFR4 is reported, and strong selectivity for FGFR4 is observed.

Quinolones can possess desirable antibacterial, antiviral and anticancer properties, rending them important synthetic targets for drug discovery purposes. Here, the gram-scale total synthesis of antiviral (+)-aniduquinolone A, possessing a 3,4-dioxygenated 5-hydroxy-4-aryl-quinolin-2(1H)-one skeleton, is reported, as well as its acid-catalyzed rearrangement to aflaquinolones A, C, and D.

Next-generation genome sequencing technologies have revolutionized the life sciences, however all sequencing platforms require nucleic acid pre-processing to generate suitable libraries for sequencing. Here, oligonucleotide-tethered 2′,3′-dideoxynucleotide terminators bearing universal priming sites are synthesised and incorporated by DNA polymerases, allowing integration of the fragmentation step into the library preparation workflow while also enabling the obtained fragments to be readily labeled by platform-specific adapters.

Identification of chiral molecules in multi-component mixtures of unknown compositions remains a challenge. Here, the authors show that microwave three-wave mixing that uses broad-spectrum fields can detect chiral molecules in enantiomeric excess without prior chemical knowledge of the sample.

Gas hydrates have an important role in environmental and astrochemistry, as well as energy materials, but the hydrate nucleation process is not fully understood. Here, the authors use molecular dynamics simulations to show that methane molecules gather with a three-body aggregate pattern.

The conversion of carbon oxides to products such as fuels is of high industrial relevance, but uncertainties regarding the catalytic mechanisms remain. Here, the authors use in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to follow CO, CO₂, H₂ and H₂O molecules as they bind to a Cu/TiO₂ surface, finding metallic copper sites serve as CO₂ dissociation sites, whereas Cu⁺ and oxygen vacancies bind CO molecules for further reductions.

The cluster approach is a very valuable technique for elucidating reaction mechanisms of enzymes. Here, the authors discuss the current status of this methodology, highlighting its strengths and weaknesses, and argue that it should be the method of choice for investigating enzymatic reaction mechanisms.

This International Women’s Day, the editors of Communications Chemistry reflect on the responsibilities that journal editors have towards promoting gender equity in STEM, and outline some of the ways in which editors can show up for women in chemistry.

Emerging experimental techniques combined with theoretical advances allow unprecedented studies of the dynamics of gas phase molecules and clusters induced in interactions with photons, electrons, or heavy particles. Here, the authors highlight recent advances, key open questions, and challenges in this field of research with focus on experimental studies of dynamics of ions stored on millisecond timescales and beyond, and its applications in astrochemistry and astronomy.

N^ε-methylation of lysine residues in histones plays an essential role in the regulation of eukaryotic transcription, and understanding the extent to which histone N^ε-methyllysine readers and erasers can manifest selectivity is of fundamental and medicinal interest. Here, the authors study the phosphonium analogue of N^ε-trimethyllysine, finding that a subtle substitution from nitrogen to phosphorus substantially affects its interactions with N^ε-methyllysine readers and erasers.

Electrically conductive two-dimensional metal–organic frameworks have emerged as promising materials for electronic and energy storage devices, but their stacked nature offers limited accessibility to the framework pores. Now, pillaring a conductive 2D MOF is shown to enhance gravimetric capacitance by more than double.

Methacrolein oxide (MACRO) is an important carbonyl oxide produced in the atmospheric ozonolysis of isoprene, but its formation is still not fully described. Here, the authors characterize the source reaction of MACRO via infrared spectroscopy and report spectra of anti-trans-MACRO as well as its associated precursor and adduct radicals.

Despite its electron deficiency, boron can form multiple bonds with a variety of elements, but such bonds between boron and main-group metal elements are relatively rare. Here, the authors characterize boron–lead multiple bonds in PbB₂O^- and PbB₃O₂^- produced by laser vaporization.

Metal–organic frameworks have demonstrated great potential as drug delivery systems, but the biocompatibility of the MOF components is often overlooked. Here, a vitamin C and zinc-based MOF with permanent microporosity is designed, and successful loading and release of model drug urea from the MOF pores, as well as degradation of the framework, are demonstrated.

Understanding the molecular interactions between proton-dependent oligopeptide transporters and their inhibitors is key to drug and tool development, but high-resolution co-crystal structure data remains scarce. Here, the authors report the crystal structure of YePEPT-K314A in complex with the potent inhibitor Lys[Z(NO₂)]-Val, revealing the molecular interactions involved in inhibitor binding and a previously undescribed hydrophobic pocket.