One-pot Research Articles

Metal-free C[sbnd]H thioarylation of uracils and in situ generated enaminones using thiols in the presence of hexachloroethane

A metal-free and one-pot procedure for thioarylation of uracils and in situ generated enaminones with thiols in the presence of C2Cl6 is introduced. This protocol is a less toxic alternative to other conventional thioarylation techniques because it uses hexachloroethane as a solid oxidant, which is stable, inexpensive, readily available and easier to work with.

One-Pot Synthesis of Fe-Norepinephrine Nanoparticles for Synergetic Thermal-Enhanced Chemodynamic Therapy.

Chemodynamic therapy (CDT) is an innovative and burgeoning strategy that utilizes Fenton-Fenton-like chemistry and specific microenvironments to produce highly toxic hydroxyl radicals (•OH), with numerous methods emerging to refine this approach. Herein, we report a coordination compound, Fe-norepinephrine nanoparticles (Fe-NE NPs), via a one-pot synthesis. The Fe-NE NPs are based on ferrous ions (Fe2+) and norepinephrine, which are capable of efficient Fe2+/Fe3+ delivery. Once internalized by tumor cells, the released Fe2+/Fe3+ exerts the Fenton reaction to specifically produce toxic •OH. Moreover, the internal photothermal conversion ability of Fe-NE NPs allows us to simultaneously introduce light to trigger local heat generation and then largely improve the Fenton reaction efficiency, which enables a synergetic photothermal and chemodynamic therapy to realize satisfactory in vivo antitumor efficiency. This proof-of-concept work offers a promising approach to developing nanomaterials and refining strategies for enhanced CDT against tumors.

Assembling phthalaldehyde and o-aminochalcones by Pd(II) catalyzed tandem reaction for synthesizing isoindoloindonole fluorophores

One-pot synthesis of isoindoloindonoles having various auxochrome, from easily available starting materials phthalaldehyde and o-aminochalcone, involving palladium(II) acetate catalysis in acetic acid is reported. A mechanism based on the formation of 2-aryl-2H-isoindol-1-ol (22) intermediate is proposed for the formation of the tetracyclic core of isoindoloindonoles. The possible intramolecular cyclization via the direct participation of the carbonyl vs the adjacent αβ-conjugated double bond was evaluated. Thus, a detailed study on how the presence of electronically different groups at the β position of chalcones affects the outcome of the cyclization reaction and the photophysical properties of the resulting isoindoloindolones is presented here. Furthermore, the core structure was determined using NMR, mass and single-crystal X-ray diffraction analysis.

Optimization of Palladium-Catalyzed One-Pot Synthesis of Functionalized Furans for High-Yield Production: A Study of Catalytic and Reaction Parameters

This study investigates the palladium-catalyzed one-pot synthesis of functionalized furans from 1,3-Dicarbonyl compounds and alkenyl bromides, focusing on various catalysts and reaction parameters. Different catalysts, including PdCl₂(CH₃CN)₂, Pd(OAc)₂, and Pd(acac)2 as well as solvents, bases, and oxidants, were systematically evaluated. PdCl₂(CH₃CN)₂ emerged as the most effective catalyst, achieving a remarkable yield of 94%. Optimal reaction conditions were identified as PdCl₂(CH₃CN)₂ in dioxane at 80 °C with K₂CO₃ as the base and CuCl₂ as the oxidant. This study also explored various 1,3-diketones including Cyclohexane-1,3-dione, 5,5-Dimethylcyclohexane-1,3-dione, 2H-Pyran-3,5(4H,6H)-dione, Cyclopentane-1,3-dione, Pentane-2,4-dione, Ethyl 3-oxobutanoate, 1,3-Diphenylpropane-1,3-dione, 1,3-Dip-tolylpropane-1,3-dione, 1,3-Bis(4-chlorophenyl)propane-1,3-dione, and 1,3-Bis(4-bromo- phenyl)propane-1,3-dione, alongside different alkenyl bromides such as allyl bromide, (E)-1-Bromo-3,4-dimethylpent-2-ene, 1-Bromo-3-methylbut-2-ene, 3-Bromocyclohex-1-ene, and (E)-1-Bromohex-2-ene. These variations demonstrated the method’s versatility and the significant impact of substituents on reactivity and reaction yield. These findings highlight the importance of optimizing reaction conditions to maximize efficiency and provide insights into improving catalytic processes for enhanced product yields.

Synthesis of Hetaryl Substituted Pyrazolo[3,4-b]Quinolinone Systems by Multicomponent Cyclocondensation Reaction

In this study, the synthesis of pyrazolo[3,4-b]quinolinone compounds was carried out via one-pot three-component reactions. These reactions proceed as domino processes, making them easier to occur than the conventional multistep organic reactions. By employing this method, new organic molecules can be synthesized in a single step, using minimal time and number of trials. In the first phase of this two-step study, heteroaromatic carbaldehydes (quinoline-8-carboxaldehyde and quinoline-4-carboxaldehyde) were prepared to be used as substrates in subsequent reactions by oxidation of 8-methylquinoline and 4-methylquinoline with selenium dioxide, a mild oxidant. In the second step, heteroaromatic carbaldehyde reacted with aminopyrazole and dimedone in anhydrous ethanol by one-pot multicomponent condensation method to synthesize six new compounds with heteryl-substituted pyrazolo[3,4-b]quinolinone ring system. The crude products were obtained in excellent yields and further purified by crystallization. The structures of the compounds, which were found to be completely pure as a result of chromatographic studies, were elucidated by spectroscopic methods and elemental analysis.

Visible-light-promoted one-pot synthesis of β-keto sulfones from aryldiazo tetrafluoroborate salts via aerobic multicomponent reaction

β-Keto sulfone is a useful structure in organic chemistry and pharmaceuticals. In the present study, we developed a highly efficient visible-light-promoted reaction to prepare β-keto sulfones under mild conditions. Synthesis was achieved via one-pot multi-component reaction of aryldiazo tetrafluoroborate salts, alkenes, and DABSO in the presence of air (O2) with rhodamine B serving as the photocatalyst. A variety of β-keto sulfones were obtained at high yields by this one-pot operation under aerobic atmosphere. This oxysulfonylation procedure has benefits such as mild reaction conditions, a wide tolerance of functional groups, and simplicity, making it a promising choice for preparing valuable β-keto sulfones.

Clustered ultra-small iron oxide nanoparticles as potential T1/T2 dual–modal magnetic resonance imaging contrast agents and application to tumor model

Many studies have been conducted on the use of ultra-small iron oxide nanoparticles (USIONs) (d < 3 nm) as potential positive magnetic resonance imaging (MRI)-contrast agents (CAs); however, there is dearth of research on clustered USIONs. In this study, nearly monodispersed clustered USIONs were synthesized using a simple two-step one-pot polyol method. First, USIONs (d = 2.7 nm) were synthesized, and clustered USIONs (d = 27.9 nm) were subsequently synthesized through multiple cross-linking of USIONs with poly(acrylic acid-co-maleic acid) (PAAMA) polymers with many -COOH groups. The clustered PAAMA-USIONs exhibited very weak ferromagnetism owing to the magnetic interaction between superparamagnetic USIONs; this was evidenced by their appreciable r1= 3.9 s‒1mM‒1and high r2/r1ratio of 14.6. Their ability to function as a dual-modal T1/T2MRI-CA in T1-weighted MRI was demonstrated when they simultaneously exhibited positive and negative contrasts in T1-weighted MRI of tumor model mice after intravenous injection. They displayed positive contrasts at the kidneys, bladder, heart, and aorta and negative contrasts at the liver and tumor.&#xD.

One-pot synthesis of dihydropyrimidinone and polyhydroquinoline derivatives with natural deep eutectic solvents (NADESs): Alternative to toxic organic solvents and environmental eco-friendly

Natural deep eutectic solvents (NADESs) have emerged as a novel class of solvents with properties reminiscent of ionic liquids while offering additional advantages in terms of cost, environmental impact, and synthesis. This article focuses on the applications of NADESs of mannose:urea and glucose:dimethylurea as inexpensive, accessible, and reusable catalysts in the synthesis of dihydropyrimidinone and polyhydroquinoline derivatives. The results demonstrate significant yields for both dihydropyrimidinones (47–99%) and polyhydroquinolines (90–97%) reactions using mannose:urea and glucose:dimethylurea as catalysts. The advantages of NADESs as catalysts include their simple and reproducible preparation, low cost, environmentally benign nature, long-term durability, and tunable properties. This NADESs can also be recovered and reused for four times without a significant loss of activity.

Synthesis of sulfone bridged 2D porphyrin assembly for enhanced photocatalytic oxygenation of sulfide

In the present work, we have synthesized sulfone-bridged tetraphenyl porphyrin, 2D polymer ‘P’ (C44H28N4OySx)n through a one-pot reaction of tetra(p-bromophenyl) porphyrin, S with sulfur powder in DMF. The polymer ‘P’ has been further reacted with erythrosine B for the fabrication of composite photocatalyst, C (C65H37N4NaOySx)n using donor– acceptor conjugation protocol. Herein, both compounds (P &amp; C) have been well characterized by MAS 13C-NMR, XPS, IR, powder XRD, TGA, SEM-EDX, UV-Vis spectra, and Cyclic Voltammetry. Due to the low HOMO-LUMO band gap energy, the applicability of the composite photocatalyst (C, 2.1 eV) has been studied in terms of oxidation of sulfide to sulfoxide. The present work shows a promising route for the development of sulfone-bridged 2D porphyrin covalent organic framework (COF) and its composite photocatalyst as well as its usage in photocatalytic sulfoxidation reaction.

Flame retardant epoxy vitrimers employing a Meldrum's acid-functionalized and phosphorus-containing bisphenol compound as the cross-linking agent for conventional epoxy

In addition to recycling and reprocessing features, designs of vitrimers possessing critical properties required for conventional cross-linked polymers are of interest. In this work, a newly designed Meldrum's acid (MA)-functionalized and phosphorus-containing bisphenol compound (P-MADV) compound is synthesized. Employing P-MADV as a curing agent, simultaneous formation of permanent and dynamic covalent linkages through one-pot reaction has been achieved in formation of flame retardant epoxy resin vitrimers. The newly synthesized P-MADV compound is an effective cross-linking agent for commercially-available epoxy resins for synthesis of flame-retardant epoxy vitrimers through the conventional cross-linking conditions and processes. The cross-linked epoxy vitrimer passes the flame test under UL 94V-0 specification contributed from the phosphorus-containing groups. The flame retardant vitrimer also exhibits a storage modulus of 1.2 GPa at 50 °C and a Tg (tanδ peak) of 185 °C, which are comparable to the values found with conventional phenolic novolac-cross-linked epoxy resin (storage modulus: 1.6 GPa; Tg: 155 °C). Without addition of catalysts for dynamic bond exchanging reaction, the cross-linked epoxy vitrimer shows stress relaxation time of 397 s at 230 °C and an activation energy of stress relaxation of 97.8 kJ mol−1. The dynamic features warrant the epoxy vitrimer being recyclable under thermally pressing at 230 °C and 16 MPa for 1 h. The recycled samples exhibit thermal and mechanical properties being comparable to the pristine resin. This work has demonstrated an attractive approach for preparation of flame retardant epoxy resin vitrimers in viewpoints of both manufacturing processes and resins properties.

Enhanced electrocatalytic CO2 reduction into formate: Unleashing the effect of engineered bimetallic oxides supported on activated carbon

The excessive concentration of anthropogenic CO2 continuously harms the atmosphere. Consequently, deploying CO2 via the electrochemical reduction approach has become a highly sought-after research thrust area. In this study, a facile, one-pot solution combustion synthesis method (SCSM) was employed for the synthesis of various mixed-metal oxides supported on porous activated carbon (SnO2-CuO@AC). The prepared materials are characterized by analytical and spectroscopic techniques. Electrochemical studies were performed for the SnO2-CuO@AC catalyst to reduce CO2 into formic acid via an electrochemical approach. The in-depth properties of the designed catalysts were analysed by theoretical calculations using FT-IR and XRD data. The SnO2-CuO@AC exhibited improved electrochemical performance with a high current density of −10.77 mAcm−2, a low overpotential of −1.29 V, a lower Tafel slope value of 100 mV/dec. The faradaic efficiency for formic acid was 78.8 % at 1.3 V vs. RHE, with high stability for 9 h. The presence of coordinated active sites and oxygen vacancies, and a lower Tafel slope, also endorses CO2 adsorption and activation, faster electron transfer and boosts CO2 reduction. The significant reactivity toward CO2 reduction is attributed to the intensity of interaction between CO2∗- and the electrocatalyst, followed by kinetic activation toward protonation to obtain the desired product.

Harnessing the Power of Sugar-Based Nanoparticles: A Drug-Free Approach to Enhance Immune Checkpoint Inhibition against Glioblastoma and Pancreatic Cancer.

Cancer cells have a high demand for sugars and express diverse carbohydrate receptors, offering opportunities to improve delivery with multivalent glycopolymer materials. However, effectively delivering glycopolymers to tumors while inhibiting cancer cell activity, altering cellular metabolism, and reversing tumor-associated macrophage (TAM) polarization to overcome immunosuppression remains a challenging area of research due to the lack of reagents capable of simultaneously achieving these objectives. Here, the glycopolymer-like condensed nanoparticle (∼60 nm) was developed by a one-pot carbonization reaction with a single precursor, promoting multivalent interactions for the galactose-related receptors of the M2 macrophage (TAM) and thereby regulating the STAT3/NF-κB pathways. The subsequently induced M2-to-M1 transition was increased with the condensed level of glycopolymer-like nanoparticles. We found that the activation of the glycopolymer-like condensed galactose (CG) nanoparticles influenced monocarboxylate transporter 4 (MCT-4) function, which caused inhibited lactate efflux (similar to inhibitor effects) from cancer cells. Upon internalization via galactose-related endocytosis, CG NPs induced cellular reactive oxygen species (ROS), leading to dual functionalities of cancer cell death and M2-to-M1 macrophage polarization, thereby reducing the tumor's acidic microenvironment and immunosuppression. Blocking the nanoparticle-MCT-4 interaction with antibodies reduced their toxicity in glioblastoma (GBM) and affected macrophage polarization. In orthotopic GBM and pancreatic cancer models, the nanoparticles remodeled the tumor microenvironment from "cold" to "hot", enhancing the efficacy of anti-PD-L1/anti-PD-1 therapy by promoting macrophage polarization and activating cytotoxic T lymphocytes (CTLs) and dendritic cells (DCs). These findings suggest that glycopolymer-like nanoparticles hold promise as a galactose-elicited adjuvant for precise immunotherapy, particularly in targeting hard-to-treat cancers.

Selection of the Compromised Operating Condition of a One-Pot Multi-Enzymatic Reaction Using Individually Immobilised Enzymes: Production of Lactofructose Syrup

Selection of the Compromised Operating Condition of a One-Pot Multi-Enzymatic Reaction Using Individually Immobilised Enzymes: Production of Lactofructose Syrup

Synthesis of 2-amino-2-deoxy-1,3-dithioglucosides as N-acetyl muramyl dipeptide analogues via organocatalyzed relay reactions

Herein, we report a novel method for highly efficient and stereoselective construction of bioactive 2-amino-2-deoxy-1,3-dithioglucosides as N-acetyl muramyl dipeptide analogues via organocatalyzed relay reactions with 3-O-acetyl-2-nitroglucal as the glycosyl donor. The method enjoys mild reaction conditions, efficient one-pot relay reaction, good to excellent yield, and broad substrate scope.

Ce-doped NiCo-layered double hydroxide based self-supporting tremella-shaped nanoflower heterostructure as efficient electrocatalyst for the oxygen evolution reaction

NiCo-layered double hydroxide (NiCo-LDH) catalysts, which indicate a profound prospect of oxygen evolution reaction (OER) under alkaline conditions, are facing great challenges in terms of low electrical conductivity, restricted by poor conductivity, limited electrochemical reaction sites, and low-density of edge sites. The authors developed a simple and convenient in-situ one-pot self-assembly method. The Ce-doped defective NiCo-LDH hexagonal nanosheets and nitrogen-doped graphene fabricated the NiCoCe-LDH/RNF electrocatalyst on the nickel foam (NF) substrate, which demonstrated excellent OER activity under alkaline conditions, only needed 299 mV overvoltage to achieve 50 mA cm−2 current intensity, could last for 6 hours at 20 mA cm−2. The highly active OER benefited from the structural advantages of the novelty three-dimensional array structure. The novel geometric structure of tremella-shaped nanoflower integrated with curved nanosheets and curled edges loaded on NF provides more electrochemical reaction sites for intermediate coordination. The nitrogen-doped reduced graphene oxide accommodated better interaction between active materials and charge carriers, enhancing the conductivity and electron transfer performance of nanostructures. The effective synergistic between the heterostructures promoted the excellent OER electrocatalytic activity of NiFeCe-LDH/RNF nanocomposites. DFT calculations at the atomic level of pristine and Ce-doped NiCo-LDH exhibited that Ce-doping can reduce the Gibbs free energy of the potential-determining step and improve the catalytic activity of OER. This work has broadened the horizons for developing simple and highly available OER electrocatalysts.

Excellent C-band microwave absorption properties of Ni@nitrogen-doped porous carbon nanocomposite via polymer bubbling technique

Nitrogen-doped porous carbon nanocomposites are highly sought-after materials for electromagnetic wave absorption due to their unique combination of electrical and magnetic properties. However, achieving optimal absorption performance within the critical C-band (4–8 GHz) frequency range remains a significant challenge. Ni@NPC nanocomposites, synthesized through the polymer bubbling technique, demonstrated exceptional microwave absorption (MWA) performance in the C-band. These materials exhibited a reflection loss (RL) of −65.20 dB at a thickness of 4.8 mm. When carbonized at 600 °C, a thickness of 2.0 mm achieved an effective absorption bandwidth (EAB) of 5.74 GHz. The remarkable absorption performance is ascribed to the combined effect of their porous composition and the addition of nitrogen dopants, which efficiently foster various microwave attenuation processes. Furthermore, the material’s effectiveness in real-world applications was evaluated using computer simulation technology (CST). This work highlights the potential of the one-pot fabrication method for developing high-performance MWA materials with practical applications.

Direct Synthesis of Artificial Esterase through Molecular Imprinting Using a Substrate-Mimicking Acylthiourea Template.

Most reported artificial esterases hydrolyze only activated esters. We here report a one-pot synthesis of artificial esterases via molecular imprinting. An acylthiourea template hydrogen bonds with 4-vinylbenzoic acid and coordinates to a polymerizable zinc complex inside a cross-linkable surfactant micelle. Double cross-linking of the micelle yields a polymeric nanoparticle catalyst that mimics a metalloenzyme to activate a water molecule for nucleophilic attack on the bound ester. The catalyst hydrolyzes both activated and unactivated esters under mild conditions with selectivity.

Ultrapure gold recovery from electronic waste as nanoparticles immobilized in hydrogel matrix

Solid-supported gold nanoparticles possess significant value as economical and eco-friendly catalysts due to their durability and reusability. Conventional methods to synthesize heterogeneous catalysts require the use of expensive gold precursors, diminishing their economic viability. Recovering gold directly as nanoparticles immobilized in a solid matrix from electronic waste (e-waste) provides a promising economic solution. However, the greater abundance of other metal ions in e-waste solutions makes this task challenging, demanding more selective approaches. This study presents a cost-effective one-pot synthesis of gold nanoparticles immobilized in a hydrogel matrix from e-waste solutions, circumventing the need for gold precursors. The fabricated hydrogel exhibits exceptionally selective gold reduction, producing well-distributed and highly pure (23.78 K) gold nanoparticles inside the hydrogel matrix. The fine control in nanoparticle diameters from 22 to 35 nm was achieved by tuning the monomer compositions of the hydrogel. These hydrogel-supported gold nanoparticles demonstrate reusable catalytic properties, indicating their potential sustainability and industrial compatibility. This approach addresses the economic challenges of synthesizing solid-supported gold nanoparticles and offers a sustainable pathway.

Trimetallic ZIFs-derived nanoarchitecture for portable wireless electrochemical determination of chlorogenic acid in natural medicine and food samples

In this paper, a novel trimetallic zeolitic imidazolate frameworks (ZnCoMn-ZIFs) was successfully synthesized by a facile one-pot method at room temperature, which was further used to prepare a triatomic site anchored in N-doped carbon (Co2MnN8@C) hybrid nanostructure via a pyrolysis method. The synthesized Co2MnN8@C was modified on the screen-printed carbon electrode, and the modified electrode was used for the portable wireless sensitive determination of chlorogenic acid (CGA) by differential pulse voltammetry. The Co2MnN8@C exhibited large surface area and excellent catalytic activity with increasing Co and Mn sites, which could selectively combine with CGA to enhance the sensitivity of the electrochemical sensor. Under the optimized conditions, the constructed sensor had wider linear ranges for CGA analysis from 0.05–10.0 μmol/L and 10.0–100.0 μmol/L with a detection limit of 0.0075 μmol/L (3S0/S). The sensor was successfully applied to detect CGA in natural medicine and food samples with satisfied recoveries. Therefore, the proposed strategy may stimulate the exploration of trimetallic ZIFs with more active sites for the development of sensitive electrochemical sensors.

Biomimetic multiscale structure with hierarchically entangled topologies of cellulose-based hydrogel sensors for human-computer interaction

The development of high-performance cellulose-based sensors with superior interfacial compatibility, flexibility, and strength has always been challenging. Drawing inspiration from the intricate multiscale hierarchy found in resilient natural materials, the incorporation of this structure into cellulose-based hydrogels using biomimetic strategies is anticipated to enhance their properties. Therefore, the cellulose/polyacrylamide (PAM) hybrid hydrogels are fabricated using the aqueous AlCl3/ZnCl2 system through an all-green one-pot method at room temperature, achieving efficient dissolution of cellulose at multiple scales and in-situ polymerization of polyacrylamide. The multiscale cellulose/PAM hydrogels achieve good interfacial compatibility, with the reinforcing mechanism being confirmed through a combination of experimental validation and atomic simulations. The findings underscore the key elements that drive the multiscale behavior of hydrogels, encompassing a range of factors such as multiple interfacial interactions, hierarchical molecular entanglements, and microskeleton reinforcement. The hydrogels exhibit satisfactory stretchability (412 %), compressive strength (1.2 MPa), conductivity (1.65 S m−1), and ultralong circulability (> 12,000 cycles), rendering them suitable for various scenarios of human-computer interaction. This work establishes a comprehensive interpretation of the strengthening mechanism in cellulose-based multiscale hierarchical structures, thereby providing novel insights for the advanced design strategies of other promising hierarchical materials.