Search Results (575)

One-pot protocols leading to target products in two or more sequential reactions, without the separation and isolation of intermediate products, are powerful synthetic tools. In fact, they surpass usual procedures based on single-step reactions in terms of efficiency, cost, and green aspects. The appeal of such methodologies is further increased with the use of catalysts, which makes the process easier and more efficient, minimizing unwanted byproducts. In this context, this paper describes three new one-pot protocols, based on an oxo-Re(V)-catalyzed Meyer–Schuster rearrangement of different secondary propargylic alcohols to the corresponding α,β-unsaturated ketones. These products, without isolation, subsequently, can undergo the 1,4-conjugate addition of a soft Gilman copper nucleophile or the intramolecular cyclocondensation with hydrazine hydrochloride to pyrazoles. Moreover, the ketone formed by the addition of a Gilman reagent can further be reduced in situ with LiAlH₄ to the corresponding secondary alcohol. The remarkable aspects of these novel procedures involving two and three one-pot consecutive steps are the high overall yields, the readily available reaction conditions, and the compatible presence of two transition metallic species in the same reaction medium. Full article

Six 9-thienyl-10-aryl-substituted 3,3,6,6-tetramethyl-decahydroacridine-1,8-diones (5a–f) were prepared by two acid-mediated routes that used the same solvent, temperature, and reaction time. In the sequential route, preformed 5,5-dimethyl-3-(arylamino)cyclohex-2-enones were reacted with a heteroaryl aldehyde and dimedone; in the corresponding one-pot route, the arylamine, heteroaryl aldehyde, and two equivalents of dimedone were combined directly. The isolated yields of the product-forming second stage were 71–75%, corresponding to calculated overall two-step yields of 58.2–68.6% after accounting for the isolated enaminone-preparation yields. These overall yields remained higher than those of the one-pot procedure (40–47%), although the sequential protocol required an additional reaction, isolation, catalyst charge, and solvent-intensive operation. Structural assignments were based on the available IR, ¹H NMR, ¹³C NMR, and EI-MS data. Tetrahydroacridinone by-products 6a–c were isolated in 13–15% yields and showed diagnostic spectral changes relative to 5a–f, including loss of the C-9 methine resonance and appearance of a strongly deshielded aromatic proton at 9.17–9.21 ppm. Within the limitations of an operational preparative comparison, the product distribution is consistent with a sequence-control interpretation in which preformation of the β-enaminone favors the 1:1:2 aldehyde/amine/dimedone product, whereas simultaneous component activation permits competing Knoevenagel, xanthene-forming, and aromatization pathways. This study provides a practical synthesis of thienyl-substituted decahydroacridine-1,8-diones and a mechanistically cautious explanation for the reduced selectivity of the one-pot process. Full article

Cationic lanthanide luminophores remain underexplored compared with their neutral analogues, despite attractive features for solution-processed electroluminescent devices. Here we report the synthesis and characterization of five europium(III) cationic complexes of the type [Eu(L^{N,N})₂(L^{O,O})₂][PF₆], where L^{N,N} = 2,2′-bipyridine, 1,10-phenanthroline, or bathophenanthroline and L^{O,O} = acetylacetonate (acac) or hexafluoroacetylacetonate (hfac). These complexes are obtained in good yield via one-pot reactions from EuCl₃·6H₂O, β-diketonates, and diimine ligands, and are confirmed by FT-IR and RAMAN spectroscopies, elemental analysis, and single-crystal X-ray diffraction to possess well-defined EuO₄N₄ coordination spheres with PF₆ counterions. UV–Vis spectra show intense ligand-centered π–π* bands below ~300 nm and weak visible tails, consistent with efficient antenna sensitization and negligible direct Eu(III) f–f absorption. All complexes exhibit characteristic Eu(III) emission between ~575 and 725 nm, dominated by the ⁵D₀ → ⁷F₂ transition near 610–620 nm for all complexes and ⁵D₀ → ⁷F_3,4 transitions for 4 and 5, with similar line patterns but markedly different intensities. Replacing acac with hfac dramatically enhances performance with the quantum yields increasing from 15–18% to 85–93%, and excited-state lifetimes from 1.01–1.53 ms to 2.50–3.25 ms. These gains are attributed to improved ligand triplet to Eu(III) ⁵D₀ energy matching and reduced multiphonon relaxation, establishing these cationic Eu(III) complexes as promising emitters for solution-processable photonic devices. Full article

Aramid nanofibers (ANFs) inherit the exceptional properties of the bulk counterparts, while introducing a large specific surface area and excellent processability. However, the strong inter-fibrillar interactions and tendency to agglomerate hinder their high-content incorporation into polymer matrices. Here, we report a one-pot reprotonation–compounding strategy for fabricating aramid nanofiber-reinforced poly(vinyl alcohol) (ANF–PVA) composite films, where the ANF dispersion was mixed with polymers during the protonation process to form a continuous 3D network in the ANF-PVA film. The optimized film with a loading of 20 wt% ANFs exhibited a tensile strength of 122.2 MPa and a toughness of 28.36 J m⁻³. Furthermore, the high ANF loading enabled versatile applications. A robust ANF-PVA hydrogel, prepared via salt-induced gelation, delivered 132% enhancement in tear strength and 38.2% increase in cyclic compressive strength compared with the PVA hydrogel. Moreover, inspired by the “brick-and-mortar” architecture of natural nacre, the fully organic ANF-PVA film was incorporated into carbon fiber/epoxy laminates, with a configuration of one nacre-inspired film per five prepreg plies, achieving a 36.5% improvement in impact toughness and minimal loss in flexural strength. This scalable reprotonation–compounding approach provides a general route for producing high-loading ANF-based composites, paving the way for the broader utilization in advanced materials. Full article

Triazole-containing poly(ester amide)s were synthesized by a one-pot Cu(I)-catalyzed click step-growth polymerization using adipate-based dipropargyl esters and in situ generated diazide monomers derived from aliphatic diamines. Two polymers differing in the length of the polymethylene segment of the diamine unit (six and ten methylene groups) were obtained with yields close to 50% and molecular weights typical of step-growth polymerizations. FTIR and NMR analyses confirmed the formation of the expected polymer structures incorporating 1,2,3-triazole rings. Despite the complexity of the repeat unit, both polymers were semicrystalline and exhibited high glass transition and melting temperatures, reflecting strong intermolecular interactions associated with amide and triazole groups. Thermal stability and processability were strongly dependent on the diamine spacer length, with the longer polymethylene segment allowing melt processing without significant degradation. The polymers displayed good in vitro cytocompatibility and were suitable for the preparation of stable nanoparticles with narrow size distributions and negative zeta potentials around −30 mV. Degradation studies revealed low hydrolytic and enzymatic degradability under physiological conditions, in contrast to previously reported polyester analogues. These results highlight the potential of triazole-based poly(ester amide)s as biocompatible materials with potential interest for biomedical applications. Full article

Silica gel polymer material with imprinted phosphate cavities was successfully obtained using one-pot sol–gel reaction. Differences in the textural properties concerning the reduction in specific area and pore size between functionalized and pristine silica gel demonstrated the presence of the phosphate moieties in the cavities. The chemical and structural characterization of the functionalized material before and after copper adsorption was performed by Fourier-transform infrared spectroscopy (FTIR) and solid-state ²⁹Si and ³¹P nuclear magnetic resonance (NMR) spectroscopy. All these measures proposed a phosphate non-covalently bound in the cavities of the silica gel and stabilized by silanol groups on the surface of the matrix. The phosphate–copper complex is removed after the metal desorption process, and the free cavities in the silica matrix can be replenished with phosphoric acid without affecting its adsorption capacity. The entire process of phosphate incorporation, copper adsorption, and metal-ligand desorption was repeated in three cycles, showing a similar metal adsorption capacity. Energy-dispersive X-ray spectroscopy (SEM-EDX) experiments were performed to monitor the presence and proportion of phosphorus and copper at each step of the phosphate loading and copper adsorption processes. These results demonstrate the feasibility of synthesizing a rechargeable polymer material with functional molded cavities with phosphate groups capable of adsorbing copper ions. Finally, this investigation represents the first approach to new materials with a rechargeable ligand system for the adsorption of heavy metals. Full article

We report the study of Cur@HKUST-1 composites, obtained through one-pot infiltration of HKUST-1 with curcumin (Cur) as a guest-sensitizing molecule. Cur features a HOMO energy above the valence band (VB) of HKUST-1, enabling modulation of the electronic structure of the host framework by introducing additional energy states within the bandgap. Structural characterization, including X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA), confirmed successful guest incorporation and preservation of HKUST-1 crystallinity. An initial Cur amount of 50% (relative to the BTC linker) was added to the synthetic mixture, and differential UV-vis analysis has shown an infiltration efficiency of 28.0%, corresponding to an infiltration degree of 14% in the Cur@HKUST-1 composite, highlighting a challenging loading process, primarily due to the size and conformations of the Cur structure. Textural analysis revealed a reduction in surface area and pore volume, consistent with a high degree of guest infiltration. Optical properties evaluated by diffuse reflectance UV-vis spectroscopy revealed new absorption bands and a notable decrease of 1.83 eV in the bandgap energy from 3.68 eV (HKUST-1) to 1.85 eV (Cur@HKUST-1) due to guest molecule infiltration. Density functional theory (DFT) calculations supported the experimental findings, showing that guest HOMOs promoted the formation of a new valence band (VB), while the original VB remains lower in energy. Density-of-states analysis confirmed that the new VB originates from 2p orbitals belonging to the guest, while the conduction band remains predominantly Cu-based from the HKUST-1 framework. Photoelectrochemical characterization revealed that the guest-modified material exhibits an enhanced photocurrent response compared to HKUST-1. Cur@HKUST-1 displayed higher stability and stronger photocurrent density, attributed to its narrower bandgap and increased charge carrier density. These results demonstrate the potential of rational guest selection to engineer band structure and improve the light-harvesting performance of MOFs in solar-driven applications. Full article

Hydrolysis of cellulose to produce ethanol has become an effective way to utilize biological resources, but its large-scale industrial application has been limited. In this study, a one-pot catalytic conversion process for transforming cellulose into ethanol was developed. Meanwhile, multifunctional Mo/Pt/WO_x/Al₂O₃ catalysts were prepared by loading nano-alumina (Nano-Al₂O₃) via a stepwise impregnation method. The influence of catalysts with varying metal ratios on the types of products generated during the cellulose hydrolysis process to ethanol was examined. The catalyst with 0.1% Mo, 2% Pt, and 7.5% W loadings showed the best selectivity. With an ethanol yield of 45.3% after heating at 5 MPa H₂ and 518 K for 2 h. Nano-Al₂O₃ can provide suitable active sites. The addition of W⁵⁺ and Mo⁰ increased the surface oxygen vacancy density and enhanced the hydrodeoxidation and metal anchoring capacity of the catalyst. The solid solution structure facilitates electron transfer from W and Mo atoms to Pt atoms, forming electron-rich Pt^δ- species, promoting the hydrolysis of cellulose and the formation of ethanol. Full article

Developing high-performance non-precious metal catalysts for the methanol oxidation reaction remains a challenge for direct methanol fuel cells. Herein, a nickel-doped Beta (Ni-Beta) zeolite was successfully synthesized via a template-free one-pot hydrothermal route followed by protonation via ammonium exchange. In this work, the protonation process strengthened metal–support interaction to form Ni²⁺/Ni³⁺ redox pairs, introduced abundant acidic sites, and optimized the zeolitic pore structure. Optimized Ni-H-Beta-170 (Si/Ni = 170) achieved a remarkable mass activity of 71.6 A g⁻¹ at 0.66 V vs. Hg/HgO, around 10-fold higher than unprotonated Ni-Beta zeolite. The improved activity originates from reversible Ni²⁺/Ni³⁺ cycles for eliminating toxic CO_ads, enriched acid sites accelerating C–H cleavage of methanol and formation of active NiOOH, and enlarged pore volume facilitating mass transfer. This work offers a low-cost strategy toward advanced non-precious methanol oxidation reaction electrocatalysts. Full article

This study presents a transformative “one-pot” biorefinery approach for the simultaneous production of hyaluronic acid (HA) and polyhydroxybutyrate (PHB) using an engineered, non-pathogenic Halomonas bluephagenesis TD01 chassis. By leveraging the principles of Next-Generation Industrial Biotechnology (NGIB), a one-step fermentation process was developed in nutrient-rich 40-LBG-Y medium, achieving a balanced metabolic flux that yielded 1.99 g/L and high-molecular-weight (HMw) HA (9.6 × 10⁶ Da) as the highest HA-Mw reported by heterogeneous bacteria, alongside intracellular PHB (0.68 to 1.6 g/L). A bioactive HA-PHB nanoparticle scaffold was fabricated, exhibiting a highly porous, interconnected 3D sponge-like architecture with a significant particle size shift from 12 nm to 450 nm, confirming successful polymer complexation. Antimicrobial evaluations revealed that the scaffold exhibited preliminary antimicrobial potential against representative Gram-positive and Gram-negative strains against Staphylococcus aureus, Klebsiella variicola, and Candida albicans. Notably, while Pseudomonas aeruginosa metabolically exploited purified HA, the integrated scaffold reversed this effect, providing preliminary antimicrobial potential by sterically hindering bacterial hyaluronidases. Furthermore, Halomonas-derived HA consistently outperformed Moringa oil and complex emulsions in preliminary tests against a wide range of pathogenic microbes. These results demonstrate that this dual-product platform provides a sustainable, cost-effective source of high-performance functional materials for advanced antimicrobial coatings and clinical wound management. Full article

Reactivity of non-aromatic 2,5-dichloro-2H-pyrroles toward S-nucleophiles was investigated. It was found that these non-aromatic derivatives exhibit both oxidative and electrophilic properties. Their reaction with thiols and xanthates proceeds as redox process to form disulfides and 5-chlorinated pyrroles as a result of 2,5-dichloro-2H-pyrroles reduction. However, the reaction with ammonium thiocyanate afforded the corresponding 5-thiocyanated 1H-pyrroles. Based on these findings, a novel one-pot method for the thiocyanation of 2,3,4-trisubstituted pyrroles was developed. The protocol involves the in situ generation of highly reactive 2,5-dichloro-2H-pyrroles via dearomative chlorination of the corresponding pyrroles using trichloroisocyanuric acid (TCCA). Subsequent addition of ammonium thiocyanate leads to regioselective incorporation of a thiocyanate group at the C5 position and rearomatization of the pyrrole core. A broad scope of pyrrole-5-thiocyanates was obtained in yields up to 82%. Furthermore, these derivatives were efficiently transformed into 5-trifluoromethylthiolated pyrroles using Ruppert’s reagent in up to 94% yield. This reaction sequence provides a cost-effective way to obtain 5-trifluoromethylthiolated pyrroles, avoiding the need for high-cost electrophilic reagents. The synthetic utility of these novel sulfur-containing pyrrole derivatives was also demonstrated. Full article

Carbamazepine (CBZ), a poorly biodegradable antibiotic, is widely detected in aquatic environments, posing potential threats to ecosystems and human health. There is an urgent need to develop efficient water treatment technologies. This study successfully prepared nitrogen-doped biochar composite materials loaded with zero-valent iron (Fe⁰@CN) via a one-pot calcination method for activating peroxymonosulfate (PMS) to degrade CBZ. The material was systematically characterized using multiple analytical techniques. Results indicate that Fe⁰@CN-1.5 exhibits a high specific surface area (482.65 m²/g) and an abundant mesoporous structure, with nitrogen doping promoting graphitic structure formation and the uniform dispersion of zero-valent iron. Under conditions of a 0.3 g/L catalyst loading, a 15 mM PMS concentration, and an initial pH of 5.5, 30 mg/L of CBZ achieved 97% degradation within 30 min. Radical quenching experiments and electrochemical analysis indicate that ·SO₄⁻ and ·OH are the primary active species in this system, alongside non-radical electron transfer processes. The material demonstrates excellent degradation performance and cycling stability across various real-world water bodies and pollutant systems. This study provides a carbon-based catalytic material with application potential and a theoretical basis for the efficient treatment of antibiotic wastewater. Full article

Background/Objectives: Protein–carbohydrate interactions are implicated in amyloid aggregation pathways associated with Alzheimer’s disease (AD). Designing glycomimetics that modulate amyloid assembly represents a promising strategy. In addition, the interaction of Aβ_1–42 oligomers (Aβo) with prion protein (PrP^C) activates Fyn kinase and leads to Tau hyperphosphorylation, another process characterizing AD. Thus, we generated a library of phenyl 2-acetamidoselenogalactoside mimetics to evaluate their interactions with Aβo and disruption of Aβo–PrP^C binding, and consequently their potential to inhibit Fyn kinase activation. Methods: The synthetic approach comprised azidophenylselenylation, a modified one-pot Staudinger reduction–acylation, a selective α-glycosylation, and deacetylation. Structural diversity was achieved mainly via acylation or ureation. The compounds were screened for binding to Aβo using STD-NMR, ¹⁹F-NMR, and rapid equilibrium dialysis (RED). ADME properties were assessed through microsomal metabolism and solubility assays, while cytotoxicity was evaluated by MTT assays in human embryonic kidney (HEK) cells. Results: Several compounds bound Aβo in STD-NMR experiments, mainly through aromatic and anomeric protons, and phenyl 2-deoxy-2-phenylureido-1-seleno-α-d-galactopyranoside (34) showed the most consistent response, with >50% increase in relative binding signal in competition assays, demonstrating also some inhibition of Aβo–PrP^C interactions (12%). Selenium at the anomeric position enhanced binding compared to sulphur and oxygen analogs. RED experiments confirmed weak binding interactions, consistent with STD-NMR results. ADME revealed that acetylated compounds undergo microsomal metabolism, whereas deacetylated derivatives displayed high aqueous solubility (>100 μM) and showed no cytotoxicity. Conclusions: Phenyl 2-acetamidoselenogalactosides are a novel class of amyloid-binding glycomimetics. Among them, 34 emerges as the most promising compound, combining favorable solubility, metabolic stability, low toxicity, and measurable interference with Aβo and Aβo–PrP^C interactions, thus supporting further developments toward therapeutic applications in AD. Full article

Zinc oxide nanoparticles (ZnO NPs) exhibit strong and broad-spectrum antibacterial properties, making them a promising agent for textile applications. However, their weak adhesion to fibers and poor washing durability have hindered practical use. In this work, we report zinc/catechol resin-based microspheres (Zn/CFRs) synthesized via a one-pot hydrothermal route and applied to cotton fabric through a pad-dry-cure process. The resulting Zn/CFRs exhibit a monodisperse spherical morphology, with zinc ions concentrated on the surface and ZnO NPs encapsulated within the resin matrix. The finished fabric demonstrates potent, non-leaching antibacterial activity, achieving over 99.99% inhibition against S. aureus, E. coli, and C. albicans, with excellent performance retention even after 50 laundering cycles. Furthermore, we observed that catechol oxidation in the Zn/CFRs proceeds slowly under UV light, which may contribute to the durable adhesion of the coating. Moreover, the functional finishing does not compromise the fabric’s tensile strength, hand feel, or breathability, which positions it favorably for scalable adoption in functional textile manufacturing. Full article

A one-pot strategy was developed for preparing a chitosan/Mg–Fe layered double hydroxide (LDH) composite by alkaline coprecipitation from an acidic chitosan solution containing Mg(II) and Fe(III) precursors, avoiding separate LDH synthesis and subsequent incorporation into chitosan. X-ray diffraction confirmed LDH formation within the chitosan matrix, and ICP analysis indicated an LDH-equivalent content of approximately 4.1 wt.% on an anhydrous basis. The composite exhibited enhanced chromate adsorption compared with both starting components. The experimental plateau adsorption capacity reached 137.4 mg/g, exceeding those of chitosan (92.2 mg/g) and Mg–Fe LDH (53.5 mg/g). Nonlinear isotherm fitting showed that Mg–Fe LDH was better described by the Freundlich model, whereas chitosan and the composite were better described by the Langmuir model. The kinetic behavior followed the pseudo-second-order equation, while Weber–Morris analysis indicated multistep uptake involving surface interaction and diffusion-related processes. In simulated groundwater containing chloride, bicarbonate, and sulfate, the composite removed 82% of Cr(VI) at 1.0 g/L. It also retained complete chromate uptake over five sorption/desorption cycles, although desorption efficiency decreased from 97.3% to 90.3%. A limitation of this study is that performance was evaluated mainly in batch systems and simplified simulated groundwater; validation with real contaminated waters and dynamic flow conditions is still required. Full article