One-pot Research Articles

Two Step One-Pot Synthesis of 7-Azaindole Linked 1,2,3-Triazole Hybrids: In-Vitro and In-Silico Antimicrobial Evaluation.

Herein, we report design, synthesis and characterization of a new library of 7-azaindole N-ethyl linked 1,2,3-triazoles containing ethylene as a spacer unit, and evaluation of all the synthesized compounds for their antimicrobial properties. Antibacterial potential was checked against two Gram positive (B. subtilis and S. aureus) and two Gram negative (E. coli and P. aeruginosa) bacterial strains while antifungal potential was assayed against two fungal strains (C. albicans and A. niger). All the tested compounds showed satisfactory antibacterial potency in comparison to reference drug ciprofloxacin with MIC values ranging from 0.0108 to 0.0432 μmol/mL. Interestingly, except two, all the target compounds showed better antifungal property as compared to the reference drug fluconazole with MIC values less than 0.0408 μmol/mL. One of the compounds exhibited two-fold better antifungal potential in comparison to fluconazole. Furthermore, in-silico ADMET and DFT studies reported drug likeness behavior and chemical reactivity parameters, respectively. The cytotoxicity results on substrate azide 3 and most potent 1,2,3-triazoles (5 d and 5 l) were found to be non-toxic.

Interwoven Trimeric Cage-Catenanes with Topological Chirality.

Catenanes have gained increasing attention for their unique features such as topological chirality. To date, the majority of works have focused on catenanes comprising monocyclic rings. Due to the lack of efficient synthetic strategy, catenanes of multiannulated monomers remain scarce. Here, we report the one-pot synthesis of an interwoven trimeric cage-catenane in high yield by dynamic imine condensation between diamine linkers of suitable length and trialdehyde panels in stoichiometry. The formation of cage-catenane is driven by the efficient 6-fold π-π stacking of panels. The monomeric cage and trimeric cage-catenane are interconvertible with reversible imine chemistry, with the latter thermodynamically being more favored. Using a topology-based statistical model, we first reveal that the formation probability of the interwoven catenane surpasses that of its chain-like isomer by 20%. When this pure mathematical model is refined by taking into account the strong template effect provided by the π-π stacking of aromatic panels, it shows that the interwoven structure emerges as the dominant species, almost ruling out the formation of the latter. Although composed of achiral cage monomers, the topological chirality of the interwoven trimeric catenane is unraveled by chiral-high-performance liquid chromatography (HPLC) and circular dichroism (CD) spectroscopy, and single-crystal X-ray diffraction (XRD) analysis of the interwoven cage-catenane also reveals a pair of two topological enantiomers. Our probability analysis-aided rationale would provide a design rationale for guiding the efficient synthesis of topologically sophisticated structures.

One-Pot Green Synthesis and Biological Evaluation of Dimedone-Coupled 2,3-Dihydrofuran Derivatives to Divulge Their Inhibition Potential against Staphylococcal Thioredoxin Reductase Enzyme.

New therapeutic leads are in global demand against multiple drug-resistant Staphylococcus aureus, as presently there is no drug of choice left to treat this pathogen. In the present work, we have designed, synthesized, and in vitro validated dimedone-coupled 2,3-dihydrofuran (DDHF)-based inhibitor scaffolds against Staphylococcal thioredoxin reductase (SaTR), a pivotal drug target enzyme of Gram-positive pathogens. Accordingly, a green multicomponent method that is both efficient and one pot has been optimized to synthesize DDHF derivatives. The synthesized DDHF derivatives were found to inhibit a purified SaTR enzyme. The best inhibitor derivative, DDHF20, inhibits SaTR as a competitive inhibitor for the NADPH binding site at low micromolar concentrations. DDHF20-capped silver nanoparticles are synthesized and characterized, and their bactericidal property has been checked in vitro. Furthermore, detailed in silico-based structure-guided functional studies have been carried out to uncover the plausible mode of action of DDHF20 as a potential anti-Staphylococcal therapeutic lead.

Multicomponent one pot synthesis of substituted pyridines with a highly active and recyclable hydrotalcite-lanthanum nanocatalyst

Herein, the synthesis of 2-amino-3,5-dicyano-6-sulfanyl pyridine derivatives has been studied due to wide applications of highly substituted pyridines. At first, Hydrotalcite (HT) with various loading amounts of lanthanum (HT-La) was synthesized. Then, their catalytic activities were investigated for the condensation reaction of benzaldehyde, malononitrile, and thiophenol under reflux condition as a model reaction. The prepared HT nanocatalyst with 10 mol% of La showed the best performance in this multicomponent reaction. In addition, the reusability of the nanocatalyst was studied and the results showed, that the prepared nanocatalyst could be reused several times with an only moderate decrease in activity. Subsequently, HT-La (10 mol%) efficiently catalyzed the one-pot condensation reaction for the synthesis of highly substituted pyridines under reflux conditions. The products were produced with excellent yields, short reaction times, and easy recyclability of the nanocatalyst.

Highly Conductive Two-Dimensional FeTHBQ/Graphene Nanocomposite as the Cathode Material for Lithium-Ion Batteries.

Constructing high-performance coordination polymer (CP) cathodes for lithium-ion batteries based on the redox reactions of both high-potential transition metal ions and high-capacity organic ligands has attracted extensive attention. However, CP cathodes suffer from structural degradation, low electrical conductivity, and sluggish diffusion kinetics, resulting in poor cycling stability and inferior rate capability. Herein, the ultrafine FeTHBQ (THBQ = tetrahydroxy-1,4-benzoquinone) CP nanoparticles in situ grew on both sides of graphene nanosheets to form the uniform two-dimensional (2D) FeTHBQ/Graphene nanocomposite with a sandwich structure via a one-pot solvothermal method. The highly conductive graphene skeleton promotes the electronic conduction and structural stability for the 2D FeTHBQ/Graphene nanocomposite. Besides, compared with bulk FeTHBQ, the primary FeTHBQ nanoparticles in the FeTHBQ/Graphene nanocomposite have smaller particle sizes with larger specific surface areas. This not only shortens the Li+ diffusion distance in the FeTHBQ crystal but also benefits Li+ transfer between the electrolyte and the electrode. In the FeTHBQ/Graphene nanocomposite, the active material of FeTHBQ manifested multiple redox centers of transition metal ions (Fe3+/Fe2+) and carbonyls (C═O/C-O-) in THBQ ligands. Owing to the enhancements of structural stability, electronic conduction, and Li+ diffusion kinetics, the 2D FeTHBQ/Graphene nanocomposite presented a high lithium-ion storage capacity of 217.2 mA h g-1 at 50 mA g-1, a fast rate capability of 79.1 mA h g-1 at 5000 mA g-1, and a stable cycling performance of 87.2 mA h g-1 at 500 mA g-1 after 100 cycles. This work sheds light on the great opportunity for optimizing the electrochemical performances of CP-based functional electrode materials by combining with conductive substrates.

Ultrabright silicon nanoparticles combined with o-phenylenediamine for ratiometric fluorescence and smartphone imaging dual-mode detection of nitrite

Nitrite (NO2−) is widely present in the natural environment and human daily life. Excessive NO2− can cause harm to the environment and human health. Herein, silicon nanoparticles (SiNPs) with a fluorescence quantum yield of up to 70 % were synthesised using a one-pot hydrothermal method and combined with the common and inexpensive o-phenylenediamine (OPD) to achieve the detection of NO2−. Upon the addition of NO2−, the blue fluorescence of the SiNPs was quenched due to static quenching and Förster resonance energy transfer (FRET), while the yellow fluorescence of benzotriazole, the reaction product of OPD and NO2−, was enhanced, resulting in the fluorescence color change from blue to yellow. Based on these phenomena, a ratiometric fluorescence sensor integrated with smartphone imaging technology was developed. This sensor is notable for its portability, cost-effectiveness, and satisfactory detection limits (0.016 μM for ratiometric fluorescence and 1.64 μM for smartphone imaging). Importantly, it demonstrates high reliability and practicability in detecting NO2− in real water and food samples. This broadens the application of SiNPs in the sensing field and introduces new possibilities for NO2− detection in complex sample matrices.

5]Helicene Based π-Conjugated Macrocycles with Persistent Figure-Eight and Möbius Shapes: Efficient Synthesis, Chiral Resolution and Bright Circularly Polarized Luminescence.

π-Conjugated chiral shape-persistent molecular nanocarbons hold great potential as chiroptical materials, though their synthesis remains a considerable challenge. Here, we present a simple approach using Suzuki coupling of a [5]helicene building block with various aromatic units, enabling the one-pot synthesis of a series of chiral macrocycles with persistent figure-eight and Möbius shapes. Single-crystal structures of 7 compounds were solved, and 22 enantiomers were separated by preparative chiral HPLC. A notable pyrene-bridged figure-eight macrocycle, with its rigid, fully π-conjugated and overcrowded structure, exhibited pure excimer emission and outstanding circularly polarized luminescence (CPL) properties, including a large dissymmetric factor (|glum| = 3.8 × 10-2) and significant CPL brightness (BCPL = 710.5 M-1cm-1). This method provides a versatile synthetic platform for producing various chiral D2-symmetric figure-eight macrocycles and singly or triply twisted Möbius macrocycles with C2 and D3 symmetry, offering tunable chiroptical properties for CPL applications.

Palladium-Catalyzed One-Pot Synthesis of N-Formylaniline Derivatives Using Oxalic Acid as a Dual Carbon Monoxide and Hydrogen Donor.

A palladium-catalyzed three-component reaction enabled the synthesis of N-formylanilines from aryl iodides, NaN3, and oxalic acid. This one-pot process involves aminocarbonylation, the Curtius rearrangement, and reduction using oxalic acid as both a carbon monoxide and hydrogen donor. The method has a broad substrate scope, tolerates various functional groups, and delivers N-formylanilines in high yields, making it a green and useful synthetic approach.

One-pot synthesis of rationally-designed flexible, robust, and hydrophobic ambient-dried molecularly-bridged silica aerogels with efficient and versatile oil/water separation applications

One-pot synthesis of rationally-designed flexible, robust, and hydrophobic ambient-dried molecularly-bridged silica aerogels with efficient and versatile oil/water separation applications

Deuterated-alkylation reagents based on sulfonium salts as cation and radical sources

Abstract The replacement of C–H bonds with more stable C–D bonds at the α-position of heteroatoms, which is the typical metabolic site for cytochrome P450, is important in drug discovery. Recently, we have developed dn (deuterated)-alkylated sulfonium salts (1a-dn), which were easily prepared by deuteration (H/D exchange reaction) with D2O of the corresponding alkyl diphenylsulfonium salts (1a), as electrophilic dn-alkylating reagents (cation sources). Herein, we newly report an improved preparation method of 1a and one-pot synthesis of dn-alkylated compounds via the deuteration of 1a with D2O and the subsequent nucleophilic substitution under basic conditions. Additionally, dn-alkyl thianthrenium salts (1b-dn) were also found to work as dn-alkylating reagents (cation sources). Furthermore, 1b-dn served as radical sources under photo-induced reaction conditions with Ir photocatalyst, Hantzsch ester, or triphenylamine to obtain various regioselectively deuterium-incorporated alkyl compounds. These dn-alkylating reagents will contribute to advance the drug discovery.

Favorable formation of needle-shaped NiAl2O4 phase over macroporous Ni/CexZr1-xO2–Al2O3 catalysts in one-pot preparation and coke-resistant catalytic performance in dry reforming of methane

In this study, we report the formation of needle-shaped NiAl2O4 via favorable interactions between Ni and Al species over macroporous Ni/CexZr1-xO2–Al2O3 catalysts for dry reforming of methane (DRM) and its remarkable improvement in the catalytic performance. The macroporous catalysts prepared by a one-pot (OP) method promote a favorable interaction between Ni and Al species that results in the formation of unique needle-shaped NiAl2O4 due to easy access to each other compared with that by incipient wetness impregnation. The NiAl2O4 phase in the calcined catalysts transforms into highly dispersed Ni and defective Al2O3 via the Ni exsolution in the reduction step. The presence of oxygen vacancies near Ni0 species facilitates the CO2 activation and enhances the catalyst stability over DRM. The optimized distribution of active sites with abundant defects over macroporous Ni/CexZr1-xO2-Al2O3 catalysts (OP) result in high conversions of CH4 and CO2 and a low coking rate in DRM.

Preparation and thermal stability research of oxalic acid dihydrate-glutaric acid/PAMPS phase change gel for solar thermal energy utilization

Thermal energy storage technology based on phase change materials (PCMs) can address the temporal and spatial mismatches in solar thermal energy conversion, thereby enhancing solar energy utilization efficiency. However, the liquid flow and poor thermal reliability of PCMs limit their large-scale application in solar thermal systems. In this study, we employ a simple “one-pot method” to prepare a form-stable and thermally reliable oxalic acid dihydrate-glutaric acid/poly 2-Acrylamido-2-methyl-1-propanesulfonic acid (OAD-GA/PAMPS) phase change gel. The OAD-GA/PAMPS phase change gel melts at 64.5 °C with a phase change enthalpy of 193.6 kJ/kg, the tensile strength is 7.707 MPa, and the compressive strength is 16.940 MPa. By incorporating 5 wt% BN particles, the thermal conductivity of OAD-GA/PAMPS phase change gel reaches 0.63 W/(m·K). After 200 heating-cooling cycles, the phase change temperature of the OAD-GA/PAMPS phase change gel remains nearly unchanged, and the phase change enthalpy decreases by only 5.7 %. The photo-thermal conversion efficiency of the OAD-GA/PAMPS phase change gel is 82.7 %. The high thermal reliability and photo-thermal conversion efficiency of the OAD-GA/PAMPS phase change gel makes it suitable for solar thermal energy storage applications.

Concentration dependent carbon nanodots: Tunable luminescent color and fluorescence excitation-wavelength dependence

Carbon nanodots (CNDs) exhibiting concentration dependent properties have been synthesized through a one-pot hydrothermal reaction process utilizing diethylenetriamine and l-aspartic acid. At solid-state or high concentrations, the CNDs display excitation-wavelength independent fluorescence (FL) emissions, while at low concentrations, they exhibit excitation-wavelength dependent FL emissions. Detailed characterization of the structure and optical properties reveals that the concentration dependent FL properties can be ascribed to the intrinsic-state luminescence of the CNDs at low concentrations and the assembled-state luminescence at solid-state/high concentrations. With the increase of concentration, the self-assembly behavior of CNDs may cause the transition from intrinsic-state dominant luminescence to assembled-state dominant luminescence, and finally lead to the red-shift of FL color. Furthermore, the CNDs@Urea composites possess adjustable room-temperature phosphorescence (RTP) from turquoise to yellow by controlling the CNDs doping concentration. CNDs with concentration dependent optical properties have shown certain potentials in the fields of cell imaging, fingerprint recognition and anti-counterfeiting applications.

Machine learning-assisted identification of potential cancer inhibitors: Multifunctional biomineralized CaCO3-polyethyleneimine nanoparticle carriers and their application in lung cancer therapy

Cancer, as a prevalent phenomenon among malignant tumors, has a late-stage diagnosis rate approaching half, significantly limiting treatment efficacy and imposing substantial physiological and psychological burdens on patients. Therefore, developing innovative therapeutic platforms that simultaneously optimize diagnostic accuracy, enhance therapeutic efficacy, and minimize side effects is a critical scientific challenge in the field of precision cancer medicine. In this study, we employed a simple and efficient one-pot synthesis method combined with polyethyleneimine (PEI)-mediated biomineralization technology to successfully prepare calcium carbonate-polyethyleneimine (CaCO3-PEI) composite nanoparticles. These nanoparticles exhibit high pH sensitivity and can rapidly degrade under the mildly acidic conditions that mimic the tumor microenvironment, providing potential for targeted tumor therapy. Subsequently, we encapsulated compound 1, which has potential for lung cancer treatment, within the CaCO3-PEI nanoparticles, successfully constructing the CaCO3-PEI@1 composite system. Structural analysis of this composite system was conducted through characterization techniques. In vitro cell experiments demonstrated that the CaCO3-PEI@1 composite system exhibited significant anticancer effects by effectively inhibiting cancer cell proliferation through the regulation of apoptosis-related protein Bax expression. This provides new insights and experimental evidence for the development of cancer treatment strategies. Based on the experiment and molecular docking identified activity against lung cancer, the compound 1 was used as the initiator for the machine learning model, and up to 10,000 episodes were generated, after thorough examination, it was found about two-thirds of the generated episodes were entirely different from each other, which demonstrated that the machine learning model was a powerful tool for designing of potential inhibitors against lung cancer.

Fluorescent Determination of Uric Acid Based on Porphyrin and ZnCo2O4 Nanocomposite.

Advances in porphyrin chemistry have provided exciting technologies in the field of optical biosensing. Herein, we have synthesized 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin (TCPP) and porous Zn0.1Co2O4 nanorods using a simple one-pot hydrothermal method. The obtained TCPP- Zn0.1Co2O4 composite was then used for the development of a novel optical sensor for the determination of uric acid (UA), which is an important biomarker in human urine, serum or saliva for the clinical diagnosis of hyperuricemia and hypouricemia, etc. TCPP-Zn0.1Co2O4 composite was characterized using SEM, TEM, EDAX, PXRD, FT-IR, UV-Visible, and NMR spectroscopic techniques. The fluorescence emission spectral analysis of TCPP-Zn0.1Co2O4 was then investigated for potential applications in the detection of uric acid via the fluorescence quenching mechanism. The designed sensor showed a linear response towards the uric acid in the concentration range of 0.99 to 5.2 nM. The optical sensor exhibits a sensitive response to uric acid with a detection limit of 0.015 nM. The sensor was employed to quantify UA in spiked human urine samples and artificial urine with satisfactory results.

Iron Single-Atom Nanozyme with Inflammation-Suppressing for Inhibiting Multidrug-Resistant Bacterial Infection and Facilitating Wound Healing.

Infection with drug-resistant bacteria and the formation of biofilms are the main factors contributing to wound healing insufficiency. Antibacterial agents with enzyme-like properties have exhibited considerable potential for efficient eradication of drug-resistant microorganisms due to their superior sensitivities and minimal side effects. In this work, we prepared a kind of Fe-centered single-atom nanozyme (Fe-SAzyme) with high biocompatibility and stability via a facile one-pot hydrothermal method, which was suitable for the treatment of wounds infected with drug-resistant bacteria. The Fe-SAzyme exhibited remarkable peroxidase-like catalytic activities, catalyzing the conversion of hydrogen peroxide (H2O2) to highly toxic hydroxyl radicals (•OH), which could not only damage bacterial cells but also inhibit, disrupt, and eradicate the formation of bacterial biofilms. Thus, Fe-SAzyme demonstrated a broad-spectrum antibacterial performance capable of effectively eliminating multidrug-resistant bacteria. The coexistence of ferrous (Fe2+) and ferric (Fe3+) ions in Fe-SAzyme conferred the nanozyme with anti-inflammatory activity, effectively suppressing excessive inflammation. Meanwhile, Fe-SAzyme could significantly downregulate inflammatory cytokines tumor necrosis factor-α and interleukin-1β and upregulate growth factors VEGF and epidermal growth factor, which can prevent bacterial infection, mitigate inflammation, promote fibroblast proliferation, and improve wound closure. Thus, Fe-SAzyme had shown favorable therapeutic efficiency in promoting bacteria-infected wound healing. This study provides Fe-SAzyme as a promising candidate for the development of new strategies to treat multidrug-resistant bacterial infections.

Green room-temperature fabrication of phosphotungstic acid functionalized MOF-808 for efficient removal of cationic antibiotics

ZrⅣ-based metal–organic frameworks (MOFs)–featuring exceptional water stability, large surface area, and structural tunability–hold promise for efficient antibiotics adsorption from water. However, their inherent positive charge in neutral environments and the harsh conditions required for their synthesis hinder their effective removal of cationic antibiotics. To address this challenge, a green one-pot synthesis approach was proposed to fabricate phosphotungstic acid-functionalized MOF-808 (termed as PTA@MOF-808) at room temperature for elevated antibiotic adsorption. This approach not only leverages the strong electronegativity of PTA to improve electrostatic interactions and π-π stacking but also finely tailors the pore size of MOF-808, resulting in enhanced adsorption capacity of PTA@MOF-808. The influence of PTA loading, solution pH, and absorbent dosage on the performance of PTA@MOF-808 were studied in detail. Adsorption experiments demonstrated that PTA@MOF-808 outperformed unmodified MOF-808 in removing various positively charged antibiotics, with 5 % PTA@MOF-808 exhibiting maximum adsorption capacities of 548.1 mg g−1 and 482.9 mg g−1, for DOX and TCHC, respectively. The adsorption process followed the Langmuir isothermal model and the pseudo-second-order kinetic equation. Furthermore, the composite PTA@MOF-808 displayed excellent reusability after multiple adsorption–desorption cycles. These findings highlight the potential of PTA@MOF-808 as a promising absorbent for removing specific antibiotics from water, with significant implications for wastewater treatment.

Detection of urea in milk by urease-inorganic hybrid nanoflowers combined with portable colorimetric microliter tube.

Asimple one-pot green synthesis method was used to prepare urease-inorganic hybrid nanoflowers (UE-HNFs), which had a high surface-to-volume ratio to improve enzyme catalytic efficiency and make urease reusable. A portable colorimetric microliter tube based on urease-inorganic hybrid nanoflowers (UE-HNFs-PCMT), as an urea colorimetric biosensor, was developed for determining urea concentration in milk. The combination of urea colorimetric biosensor and asmartphone is usedfor capturingthe colour change of milk after reaction. There was a good linear relationship between colour intensity of the image (Δ intensity) and urea concentration (43-600mg L-1), with a detection limit of 12.81mg L-1. UE-HNFs-PCMT has the advantages of no need for complex equipment, easy operation, reusability, low detection cost, good portability, and environmental friendliness and can achieve urea detection in milk.

Robust conductive hydrogel advances self-powered intelligent sports monitoring and fair judging

Currently, combining multimodal perceptual ability with mechanical robustness poses a significant challenge for developing hydrogel-based flexible electronics. Herein, a robust conductive hydrogel was successfully synthesized by introducing cellulose nanocrystals (CNC) as nanofillers and lithium chloride (LiCl) as the conductive component into the copolymer network through a one-pot crosslinking procedure in a water-dimethyl sulfoxide binary solvent. Besides excellent stretchable, self-adhesive, anti-freezing, self-healing, and anti-swelling properties, tunable and reversible optical property was realized due to the polarity-induced microphase separation of the hydrophilic and hydrophobic group in the zwitterionic sulfobetaine chains, enabling cyclic information encryption and decryption. An all-weather wearable sensor array was thus developed for multi-modal sensing of various environmental stimuli, including mechanical, and thermal variations. Specifically, the intensity and spatial distribution of strain can be detected almost in real time within a broad strain range, thus realizing speech recognation, text-to-speech and human electrocardiogram signal acquisition and underwater non-contact sensing functions. Notably, the CPAMD-based triboelectric nanogenerator demonstrates impressive temperature tolerance (−40 °C and 60 °C), and remarkable material identification capability. A non-contact proximity sensing sensor and a foul detection system were thus developed by coupling the piezoresistive, triboelectric and capacitive sensing metrics to serve as an electronic referee for identifying foul in curling. This work provides a valuable reference toward combining excellent mechanical robustness with balanced electrical performance for tactile perception and intelligent sports monitoring.

Carbonylative Cyclization of 2-Iodofluorobenzenes and 2-Aminophenols with Recyclable Palladium-Complexed Dendrimers on SBA-15: One-Pot Synthesis of Dibenzoxazepinones.

A novel, efficient, and practical route to dibenzoxazepinones has been developed through a one-pot heterogeneous palladium-catalyzed aminocarbonylation/aromatic nucleophilic substitution (SNAr) sequence starting from readily available 2-iodofluorobenzenes and 2-aminophenols. The carbonylative cyclization reaction proceeds smoothly in dimethyl sulfoxide (DMSO) at 120 °C with 1,8-diazabicyclo(5.4.0)undec-7-ene (DBU) as the base by using a polyamidoamine (PAMAM)-dendronized SBA-15-supported bidentate phosphine-palladium complex [G(1)-2P-Pd(OAc)2-SBA-15] as the catalyst under 10 bar of CO, yielding a wide variety of dibenzo[b,e][1,4]oxazepin-11(5H)-one derivatives in good to excellent yields. Moreover, this new heterogenized dendritic palladium catalyst has competitive advantages in that it can be facilely recovered by simple filtration in air and recycled more than eight times without any significant loss of activity. The broad substrate scope, high functional group tolerance, and excellent palladium catalyst recyclability of the reaction make this approach a general, efficient, and economical method for the construction of valuable dibenzoxazepinone derivatives.