Base-Promoted Ring-Opening Hydroxylation of Cyclic Sulfonium Salts.

Herein, we reported a general strategy for the synthesis of sulfur-containing primary alcohol derivatives by base-promoted ring-opening hydroxylation of cyclic sulfonium salts. A variety of sulfonium salts were successfully transformed into the desired hydroxylated products in moderate to excellent yields with good functional group tolerance. Moreover, the one-pot synthesis, scale-up reaction, and late-stage functionalization of complex molecules demonstrated the practicability of this synthetic protocol in the field of synthetic chemistry.

Biomimetic Electronic Skin through Hierarchical Polymer Structural Design.

Human skin comprises multiple hierarchical layers that perform various functions such as protection, sensing, and structural support. Developing electronic skin (E-skin) with similar properties has broad implications in health monitoring, prosthetics, and soft robotics. While previous efforts have predominantly concentrated on sensory capabilities, this study introduces a hierarchical polymer system that not only structurally resembles the epidermis-dermis bilayer structure of skin but also encompasses sensing functions. The system comprises a polymeric hydrogel, representing the "dermis", and a superimposed nanoporous polymer film, forming the "epidermis". Within the film, interconnected nanoparticles mimic the arrangement of interlocked corneocytes within the epidermis. The fabrication process employs a robust in situ interfacial precipitation polymerization of specific water-soluble monomers that become insoluble during polymerization. This process yields a hybrid layer establishing a durable interface between the film and hydrogel. Beyond the structural mimicry, this hierarchical structure offers functionalities resembling human skin, which includes (1) water loss protection of hydrogel by tailoring the hydrophobicity of the upper polymer film; (2) tactile sensing capability via self-powered triboelectric nanogenerators; (3) built-in gold nanowire-based resistive sensor toward temperature and pressure sensing. This hierarchical polymeric approach represents a potent strategy to replicate both the structure and functions of human skin in synthetic designs.

N-Terminal Lysozyme Conjugation to a Cationic Polymer Enhances Antimicrobial Activity and Overcomes Antimicrobial Resistance.

Microbial resistance to antibiotics is one of the greatest global healthcare challenges. There is an urgent need to develop effective strategies to overcome antimicrobial resistance. We, herein, report photoinduced in situ growth of a cationic polymer from the N-terminus of lysozyme. The attachment of the cationic polymer improves the proteolytic and thermal stability of lysozyme. Notably, the conjugate can efficiently overcome lysozyme resistance in Gram-positive bacteria and antibiotics-resistance in Gram-negative bacteria, which may be ascribed to the synergistic interactions of lysozyme and the cationic polymer with the bacteria to disrupt their cell membranes. In a rat periodontitis model, the lysozyme-polymer conjugate not only greatly outperforms lysozyme in therapeutic efficacy but also is superior to minocycline hydrochloride, which is the gold standard for periodontitis therapy. These findings may provide an efficient strategy to dramatically enhance the antimicrobial activities of lysozyme and pave a way to overcome antimicrobial resistance.

Synthesis of 1,2-Diamines from Vinyl Sulfonium Salts and Arylamines.

A procedure for the synthesis of 1,2-diamines from vinyl sulfonium salts and arylamines under mild conditions was developed. This present synthetic protocol not only obviates the need for a transition-metal catalyst and an oxidizing reagent but also features a broad substrates scope. The practicability of this protocol is demonstrated by the one-pot synthesis, a scale-up reaction, and transformations of the products to diverse N-heterocyclic compounds. Mechanistic studies indicate that the formation of aziridine plays a key role during this diamination process.

Two plus One: Combination Therapy Tri-systems Involving Two Membrane-Disrupting Antimicrobial Macromolecules and Antibiotics.

The escalating issue of multidrug-resistant (MDR) bacteria indicates the urgent need for new and effective strategies to combat this global health challenge. Here, we describe a new combinatorial approach that can be put forward for experimental therapy application against MDR bacteria. Specifically, we have developed a tri-system that includes the coadministration of two different membrane-disrupting-type antimicrobial agents─a synthetic antimicrobial polymer P and an antimicrobial peptide (AMP) colistin methanesulfonate (Col)─in conjunction with an antibiotic [doxycycline (Dox), rifampicin (Rif), or azithromycin (Azi)]. Traditionally, the administration of membrane-disrupting antimicrobial agents causes toxicity, but, in comparison, we demonstrated synergy and biocompatibility using this combinatorial approach. Checkerboard assays showed the occurrence of synergistic interactions in Col-Dox-P, Col-Rif-P, and Col-Azi-P tri-systems against wild-type and MDR Pseudomonas aeruginosa, with the Col-Dox-P system being the most effective. The ability to synergize thus enables the use of a lower dosage in combinations compared to the standalone agents. The tri-systems not only demonstrated bacteriostatic activity but were also bactericidal. For example, the Col-Dox-P system (at 8, 4, and 8 µg mL-1, respectively) and the Col-Rif-P system (at 4, 8, and 16 µg mL-1, respectively) were able to kill >99.999% of planktonic P. aeruginosa cells within 3 h of treatment. More importantly, an improvement of the therapeutic/selectivity index was achieved via combination therapy. Taking the Col-Dox-P system as an example, its biocompatibility with murine embryonic fibroblast cells was found to be comparable to that of polymer P alone despite the synergistic enhancement in antimicrobial activity of the combination. This resulted in a significant increase in selectivity by 16-fold for the Col-Dox-P combination system compared to P alone. Furthermore, the broad applicability of this tri-system strategy was demonstrated via the successful application of the AMP melittin in place of Col or P. Overall, this study sheds new insights on the application of membrane-disrupting antimicrobial agents in combination therapy and their potential for safer clinical use. Additionally, the information gathered in this study could inform the development of future combination therapy systems involving the simultaneous employment of multiple AMPs with antibiotics.

Changes of structures and biosynthesis/hydrolysis-associated genes expression of glucans at different Volvariella volvacea maturity stages.

In the present study, effects of maturity stage on structural characteristics and biosynthesis/hydrolysis-associated genes expression of glucans from Volvariella volvacea fruit body were well investigated. Elongation and pileus expansion stages decreased total soluble carbohydrate and protein contents to 17.09 mg/g and 8.33 mg/g, and significantly accumulated the total amino acids contents to 32.37 mg/g. Yields of crude polysaccharides significantly increased to 8.12% at egg stage and decreased to 3.72% at pileus expansion stage. Purified VVP I-a and VVP I-b were proved to be α-glucans. The maturity process affected the monosaccharide compositions, decreased the molecular weights of VVP I-a and VVP I-b with decreased transcription levels of glucan biosynthesis-associated enzyme genes vvugp and vvgls and increased glucan hydrolysis-associated glucanase gene vvexg2 expression with no significant effects on backbone structures including glycosidic linkages and configurations. The findings would benefit for understanding change patterns of V. volvacea glucan structures and their biosynthesis/hydrolysis-associated genes expression at maturity stages.

Amperometric hydrogen peroxide sensor using a glassy carbon electrode modified with a nanocomposite prepared from ferumoxytol and reduced graphene oxide decorated with platinum nanoparticles.

A high-performance electrochemical H2O2 sensor was prepared by constructing multiple interfaces using platinum nanoparticles (Pt NPs), ferumoxytol (Fer) and reduced graphene oxide (rGO) on a glassy carbon electrode (GCE). The morphology of Fer/rGO and Fer/rGO-Pt was characterized by field emission scanning electron microscopy and energy-dispersive X-ray spectroscopy. Cyclic voltammetry and chronoamperometry were adopted to characterize the electrochemical properties of the sensor. Because of the synergistic catalytic effect of the compositions (rGO, Fer and Pt NPs) on the multiple interfaces, the sensor exhibits particularly high electrocatalytic activity toward the reduction of H2O2 with a low detection limit (~0.38 µM), a linear range (0.0004-0.01, 0.0075-4.3 and 4.9-10.8 mM), and a high sensitivity (340 µA mM-1 cm-2, n = 4) operated at a typical working voltage of +0.1 V (vs. Ag/AgCl). The electrode is selective and long-term stable. It was successfully applied to the determination of H2O2 in (spiked) milk samples. Graphical abstract Schematic presentation of an electrochemical H2O2 sensor using platinum nanoparticles (Pt NPs), ferumoxytol (Fer) and reduced graphene oxide (rGO) nanocomposites modified glassy carbon electrode (GCE). The sensor was applied to the determination of H2O2 in (spiked) milk samples.

Selective, Sensitive and Label-Free Detection of Fe3+ Ion in Tap Water Using Highly Fluorescent Graphene Quantum Dots.

Graphene quantum dots (GQDs) as a new type of fluorescent carbon nanomaterials, showing excellent photoluminescence properties, biocompatibility, photoelectric properties, have become the current research focus. Iron element as an essential element in the human body and an important part of hemoglobin, is very important for human health, so the detection of ferric ions has great significance. In this paper, GQDs with strong blue light emission were prepared through pyrolysis treatment using citric acid as a carbon source. Through characterization by transmission electron microscopy (TEM) and fluorescence spectrometer, it was observed that the GQDs have a uniform particle size distribution and highly fluorescent intensity with a quantum yield of 27.4%. Due to the strong quenching effect of Fe3+ on GQDs fluorescence, GQDs was used as a green and facile fluorescence sensor to detect Fe3+ selectively and sensitively. The GQDs fluorescence sensor shows a sensitive response to Fe3+ in a wide linear range (3.5 × 10-6-6.7 × 10-4 M), a low detection limit of 1.6 µM (S/N = 3) and good selectivity. Importantly, the new sensor realizes the detection of Fe3+ ions in tap water because of its low detection limit, wide linear range, and high sensitivity.