Synthesis–Structure–Property Relationships for Hyperbranched Aminosilica CO2 Adsorbents

Hyperbranched aminosilica (HAS) adsorbents are prepared via the ring‐opening polymerization of aziridine in the presence of mesoporous silica SBA‐15 support. The aminopolymers are covalently bound to the silica support and capture CO₂ reversibly in a temperature swing process. Here, a range of HAS materials are prepared with different organic loadings. The effects of organic loading on the structural properties and CO₂ adsorption properties of the resultant hybrid materials are examined. The residual porosity in the HAS adsorbents after organic loading, as well as the molecular weights and degrees of branching for the separated aminopolymers, are determined to draw a relationship between adsorbent structure and performance. Humid adsorption working capacities and apparent adsorption kinetics are determined from experiments in a packed‐bed flow system monitored by mass spectrometry. Dry adsorption isotherms are presented for one HAS adsorbent with a high amine loading at 35 and 75 °C. These combined results establish the relationships between adsorbent synthesis, structure, and CO₂ adsorption properties of the family of HAS materials.     

Apparent solubility of lycopene and β-carotene in supercritical CO2, CO2 + ethanol and CO2 + canola oil using dynamic extraction of tomatoes

Lycopene and β-carotene were extracted from freeze-dried tomatoes (skin + pulp) with pure SC CO₂ and SC CO₂ + 5% w/w co-solvent at 40 °C, 400 bar and flow rates of 0.5 and 1.2 L/min. The apparent solubility of lycopene and β-carotene in the multicomponent complex system was determined from dynamic extraction experiments using a laboratory-scale supercritical extraction system. Solubility of pure lycopene and β-carotene in SC CO₂ (binary system) was reported in the literature to be of the order of 10⁻⁶ mole fraction. The apparent solubility of lycopene extracted from tomatoes with SC CO₂ (multicomponent complex system) under the same conditions was almost one order of magnitude smaller. The apparent solubility obtained using oil as a co-solvent was higher than that obtained with ethanol as a co-solvent or pure SC CO₂. The differences in solubility are mainly due to the polarity of the co-solvent and the impact of the tomato matrix in the multicomponent complex system.     

Bactericidal paper impregnated with silver nanoparticles for point-of-use water treatment

There is an urgent need for cheap point-of-use methods to purify drinking water. We describe a method to deactivate pathogenic bacteria by percolation through a paper sheet containing silver nanoparticles. The silver nanoparticles are deposited by the in situ reduction of silver nitrate on the cellulose fibers of an absorbent blotting paper sheet. The aim is to achieve inactivation of bacteria during percolation through the sheet, rather than removal of bacteria from the effluent by filtration. The silver-nanoparticle containing (AgNP) papers were tested for performance in the laboratory with respect to bacteria inactivation and silver leaching as suspensions of bacteria percolated through the paper. The AgNP sheets exhibited antibacterial properties toward suspensions of Escherichia coli and Enterococcus faecalis, with log reduction values in the effluent of over log 6 and log 3, respectively. The silver loss from the AgNP sheets was minimal, with values under 0.1 ppm (the current US EPA and WHO limit for silver in drinking water). These results show promise that percolation of bacterially contaminated water through paper embedded with silver nanoparticles could be an effective emergency water treatment.     

Front Cover: Development and Characterization of Selective FAK Inhibitors and PROTACs with In Vivo Activity (ChemBioChem 19/2023)

Focal adhesion kinase (FAK) is an attractive drug target due to its overexpression in cancer. FAK functions as a non-receptor tyrosine kinase and scaffolding protein, coordinating several downstream signaling effectors and cellular processes. While drug discovery efforts have largely focused on targeting FAK kinase activity, FAK inhibitors have failed to show efficacy as single agents in clinical trials. Here, using structure-guided design, we report the development of a selective FAK inhibitor (BSJ-04-175) and degrader (BSJ-04-146) to evaluate the consequences and advantages of abolishing all FAK activity in cancer models. BSJ-04-146 achieves rapid and potent FAK degradation with high proteome-wide specificity in cancer cells and induces durable degradation in mice. Compared to kinase inhibition, targeted degradation of FAK exhibits pronounced improved activity on downstream signaling and cancer cell viability and migration. Together, BSJ-04-175 and BSJ-04-146 are valuable chemical tools to dissect the specific consequences of targeting FAK through small-molecule inhibition or degradation.     

Research software engineering and the importance of scientific models

Software and Systems Modeling -     

Nucleotide-Driven Molecular Sensing of Monkeypox Virus Through Hierarchical Self-Assembly of 2D Hafnium Disulfide Nanoplatelets and Gold Nanospheres

Liquid interfaces facilitate the organization of nanometer-scale biomaterials with plasmonic properties suitable for molecular diagnostics. Using hierarchical assemblage of 2D hafnium disulfide nanoplatelets and zero-dimensional spherical gold nanoparticles, the design of a multifunctional material is reported. When the target analyte is present, the nanocomposites’ self-assembling pattern changes, altering their plasmonic response. Using monkeypox virus (MPXV) as an example, the findings reveal that adding genomic DNA to the nanocomposite surface increases the agglomeration between gold nanoparticles and decreases the π-stacking distance between hafnium disulfide nanoplatelets. Further, this self-assembled nanomaterial is found to have minimal cross-reactivity toward other pathogens and a limit of detection of 7.6 pg µL⁻¹ (i.e., 3.57 × 10⁴ copies µL⁻¹) toward MPXV. Overall, this study helped to gain a better understanding of the genomic organization of MPXV to chemically design and develop targeted nucleotides. The study has been validated by UV–vis spectroscopy, X-ray diffraction, scanning transmission electron microscopy, surface-enhanced Raman microscopy and electromagnetic simulation studies. To the best knowledge, this is the first study in literature reporting selective molecular detection of MPXV within a few minutes and without the use of any high-end instrumental techniques like polymerase chain reactions.     

A domain-specific modeling milestone

Software and Systems Modeling -     

The wild-west of modeling (Revisited)

Software and Systems Modeling -     

Chronic Effects of a High Sucrose Diet on Murine Gastrointestinal Nutrient Sensor Gene and Protein Expression Levels and Lipid Metabolism

The gastrointestinal tract (GIT) plays a key role in regulating nutrient metabolism and appetite responses. This study aimed to identify changes in the GIT that are important in the development of diet related obesity and diabetes. GIT samples were obtained from C57BL/6J male mice chronically fed a control diet or a high sucrose diet (HSD) and analysed for changes in gene, protein and metabolite levels. In HSD mice, GIT expression levels of fat oxidation genes were reduced, and increased de novo lipogenesis was evident in ileum. Gene expression levels of the putative sugar sensor, slc5a4a and slc5a4b, and fat sensor, cd36, were downregulated in the small intestines of HSD mice. In HSD mice, there was also evidence of bacterial overgrowth and a lipopolysaccharide activated inflammatory pathway involving inducible nitric oxide synthase (iNOS). In Caco-2 cells, sucrose significantly increased the expression levels of the nos2, iNOS and nitric oxide (NO) gas levels. In conclusion, sucrose fed induced obesity/diabetes is associated with changes in GI macronutrient sensing, appetite regulation and nutrient metabolism and intestinal microflora. These may be important drivers, and thus therapeutic targets, of diet-related metabolic disease.