One-pot Research Articles

Composite Hydrogels with Rapid Self-Healing, Stretchable, Moldable and Antibacterial Properties Based on PVA/ε-Poly-l-lysine/Hyaluronic Acid

Self-healing, stretchable, and moldable hydrogels have a great potential application in tissue engineering and soft robotics. Despite great success in reported hydrogels, it is still a great challenge to construct the moldable hydrogels with an ultrafast self-healing performance. Herein, the composite hydrogels (PBLH) with ultrafast self-healing, stretchable, and moldable properties were successfully constructed by poly (vinyl alcohol) (PVA), borate (B), ε-poly-l-lysine (EPL), and hyaluronic acid (HA) based on an efficient one-pot method. Fourier transform infrared spectroscopy, X-ray diffraction, and rheological measurements confirmed the formation of a dynamic network among PVA, B, EPL, and HA through the cross-linking of dynamic borate bonds, electrostatic interaction, and hydrogen bonding. Having fabricated the dynamic network structure, the damage gap of the composite hydrogels can heal within 1 min, presenting an excellent self-healing ability. Simultaneously, the composite hydrogels can be molded into various shapes, and the length of the composite hydrogels can be stretched to 15 times their original length. In addition, the composite hydrogels exhibited an excellent antibacterial property against Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli). Our results illustrated that the composite hydrogels not only retain the advantages of traditional hydrogels but also possess ultrafast self-healing, outstanding stretchable and antibacterial properties, presenting a prospective candidate for constructing biomedical materials.

Efficient fabrication of conductive sponges for wearable flexible sensors

In recent years, flexible and wearable sensors, particularly piezoresistive sensors, have been widely used in various fields such as human–computer interface, soft robotics, and artificial electronic skin. Three-dimensional (3D) conductive sponges have attracted widespread attention due to their excellent sensor performance, ease of manufacture, and seamless integration into circuits. Polydimethylsiloxane (PDMS) is widely used as an ideal substrate for these 3D conductive sponges due to its excellent chemical stability, good biocompatibility, and ideal mechanical properties. In this study, we synthesize a series of conductive silicone sponges (PCSs) by the one-pot thiol oxidative coupling reaction using commercially available multi-walled carbon nanotubes and poly((thiopropyl)methyl dimethylsiloxane). The PCSs possess controllable density and electrical conductivity. Moreover, the PCS-a sponge exhibits a wide pressure sensing range from 0.5 to 230 kPa with high-pressure sensitivity along with excellent mechanical and sensing stability. Pressure sensors fabricated using PCSs can be utilized in speech recognition systems and human activity monitoring such as arm/finger bending or walking while attached to joint positions. Additionally, they can also function as compressible switching devices for pressure alarms and LEDs.

Zirconium/niacin metal-organic framework preparation, characterization and assessment as a catalyst in one-pot synthesis of xanthene-1,8-dione derivatives with docking validation as anti-inflammatory

The zirconium/niacin metal-organic framework (MOF) was prepared by an efficient solvothermal method and the nanostructure of MOF was identified by IR, SEM, EDX, XRD, BET and TEM. The prepared Zr-MOF was evaluated as a catalyst in organic synthesis. Tetrahydro xanthene-1,8‑dione derivatives were synthesized by a one-pot reaction between 2 mol of dimedone and 1 mole of aromatic aldehyde in the presence of the catalytic amount of Zr-MOF under solvent-free conditions. The prepared ligands were evaluated as COX-1 and COX-2 inhibitors and the data obtained explained that the ligands 4-(3,3,6,6-tetramethyl-1,8-dioxo-2,3,4,5,6,7,8,9-octahydro-1H-xanthen-9-yl)phenyl benzoate (3 g), 3,3,6,6-tetramethyl-9-(5-methylfuran-2-yl)-3,4,5,6,7,9-hexahydro-1H-xanthene-1,8(2H)‑dione (3i) and 9-(3-(4-chlorophenyl)-1-phenyl-1H-pyrazol-4-yl)-3,3,6,6-tetramethyl-3,4,5,6,7,9-hexahydro-1H-xanthene-1,8(2H)‑dione (3j) gave the promised data.

Facile one-pot synthesis of CuO–Bi2O3/MgAl2O4 catalyst and its performance in the ethynylation of formaldehyde

The CuO–Bi2O3/MgAl2O4 catalyst was synthesized via one-pot synthesis and used to catalyze formaldehyde (HCHO) ethynylation. Coprecipitation using Cu2+, Bi3+, Mg2+, and Al3+ nitrates and NaOH generated Cu and Bi oxides and spinel MgAl2O4 phase. The catalyst precursor was calcined at 450 °C. The catalytic performance of CuO–Bi2O3/MgAl2O4 in the synthesis of 1,4-butynediol via HCHO ethynylation was investigated. The presence of a new spinel phase enhanced the acid–base properties on the catalyst surface and prevented the aggregation of CuO particles. These properties resulted in improved CuO dispersion during calcination and CuO particle growth suppression, affording smaller CuO crystals. The MgAl2O4 support facilitated the reduction of Cu2+ to Cu+ and formation of abundant active species during the reaction. The catalyst exhibited abundant weakly basic, fewer strongly basic, and least acidic sites, which facilitated the adsorption of HCHO and acetylene. The catalytic performance of CuO–Bi2O3/MgAl2O4 demonstrated 97 % conversion and 80 % selectivity after the online monitoring of the ethynylation reaction for 6 h. The leaching of Cu during the reaction, as analyzed by inductively coupled plasma spectroscopy, was extremely low. Moreover, conversion and selectivity did not substantially change after eight cycles. In addition, the catalyst exhibited superior activity and long-term stability in the ethynylation reaction.

Synthesis of bifunctional copolymeric nanofibers with selective extracting U(VI) from the solution and antibacterial property

Facing the problem of future nuclear fuel shortage, developing high-performance adsorbent materials is key. In this work, the amidoxime group/imidazole functionalized ionic liquid copolymer fibers containing bromide salts, and fluoroborate salts (namely P(AO/VEIMBr)8 and P(AO/VEIMBF4)6) were prepared by a one-pot method and free radical polymerization, hydroxyl amination reaction and electrostatic spinning, and characterized by SEM, FT-IR, and 1 H NMR. The influence of solid-liquid ratio, ionic strength, and adsorption time on the adsorption performance was investigated by batch adsorption experiments. In the meanwhile, the adsorption kinetics and thermodynamic processes of U(VI) on the copolymer fibers was also studied. Adsorption mechanism of U (VI) on polymer fibers was explored by XPS spectroscopic analysis combined with DFT method. Finally, the antimicrobial properties of the copolymer fibers were tested. The experimental results showed that the polymer nanofibers synthesized for U(VI) has a fast adsorption, high adsorption capacity at ionic strength close to seawater, and excellent reusability. The adsorption process conformed to the pseudo-second-order kinetic model and Langmuir model, which indicated that chemical adsorption and monolayer adsorption are dominant for adsorption U(VI) on the polymer nanofibers, and exhibits the highest Uranium adsorption capacity (76.92 mg/g and 81.96 mg/g at pH=8.1+0.1, respectively). XPS result showed the amine nitrogen and oxime oxygen in the amidoxime functional group were coordinated with uranyl(VI) ions. The antibacterial experiments showed that the copolymer fibers have antimicrobial properties and the antibacterial rate is over 90 %. Therefore, the nanofibers may be a promising material for extracting uranium from the weak alkaline wastewater or seawater.

Magnetic BiFeO3 nanoparticles: a robust and efficient nanocatalyst for the green one-pot three-component synthesis of highly substituted 3,4-dihydropyrimidine-2(1H)-one/thione derivatives.

In this research, magnetic bismuth ferrite nanoparticles (BFO MNPs) were prepared through a convenient method and characterized. The structure and morphological characteristics of the prepared nanomaterial were confirmed through analyses using Fourier-transform infrared (FTIR) spectroscopy, field emission scanning electron microscopy (FESEM), energy-dispersive X-ray spectroscopy (EDS), elemental mapping, powder X-ray diffraction (XRD), N2 adsorption-desorption isotherms and vibrating sample magnetometry (VSM) techniques. The obtained magnetic BFO nanomaterial was investigated, as a heterogeneous Lewis acid, in three component synthesis of 3,4-dihydropyrimidin-2 (1H)-ones/thiones (DHPMs/DHPMTs). It was found that the BFO MNPs exhibit remarkable efficacy in the synthesis of various DHPMs as well as their thione analogues. It is noteworthy that this research features low catalyst loading, good to excellent yields, environmentally friendly conditions, short reaction time, simple and straightforward work-up, and the reusability of the catalyst, distinguishing it from other recently reported protocols. Additionally, the structure of the DHPMs/DHPMTs was confirmed through 1H NMR, FTIR, and melting point analyses. This environmentally-benign methodology demonstrates the potential of the catalyst for more sustainable and efficient practices in green chemistry.

Photothermal synergistic catalytic oxidation mechanism of toluene by Ce-doped SrTiO3 via one-pot hydrothermal synthesis

Industrial volatile organic compounds (VOCs) emissions pose significant environmental and human health risks, with photothermal catalysis degradation emerging as a promising VOCs treatment technology. The light response range and catalysis degradation efficiency of photocatalysts, however, need to be improved. This study prepared Ce-doped SrTiO3 perovskite catalysts via a one-pot hydrothermal method. The synergistic photic/thermal degradation mechanism of toluene was uncovered via XPS, Uv–Vis, EPR, and in-situ DRIFTS analysis. It was found that the toluene removal rate and CO2 yield reached their maximums at 200 °C, reaching 95 % and 90 %, respectively, at a Ce doping ratio of 50 %. During the catalytic process, the prerequisite to trigger toluene oxidation, and light promote the generation of reactive oxygen species (·OH and ·O2–), which facilitates the formation of intermediates and thus accelerates the deep oxidation of toluene. The doped Ce increases surface oxygen vacancies while lowering the energy band gap of the catalyst, facilitating the separation of holes and photogenerated electrons. Furthermore, in situ DRIFTS studies demonstrated that toluene undergoes a ring-opening process, producing intermediates such as benzaldehyde and benzoic acid. This study will assist in promoting the use of photothermal synergistic catalytic degradation technology to remove VOCs from industrial sources.

Unprecedented one-pot synthesis of 3,4-dihydropyrimidine-2-(1h)-ones catalyzed by hydrazine sulfate through Biginelli reaction, ADMET property, molecular docking studies and their antibacterial activity on Bacillus brevis and E. coli

The syntheses of 3,4-dihydropyrimidin-2(1H)-ones by one-pot, three-component condensation of aldehydes, β-ketoesters and urea or thiourea have been made more simple and efficient by using 20 mol% hydrazine sulfate as catalyst. Aldehydes, β-ketoesters and urea are cyclocondensed in the presence of hydrazine sulfate to produce dihydropyrimidines in ethanol under reflux conditions. The advantages of using hydrazine sulfate as a catalyst over the traditional Biginelli reaction conditions include outstanding yields (80–91%) and a shorter (10–15 hours) reaction time. In order to evaluate the antibacterial efficiencies of the synthesized compounds, we have studied the inhibitions of microbial proliferation of both Gram-positive (Bacillus brevis) and Gram-negative (E. coli) bacterial strains in comparison to a control group. The microbial inhibitions occur in the range of 40–98% by different derivatives of dihydropyrimidinones. Molecular docking studies of the synthesized compounds have also been done using software tools such as SwissADME.

Rh nanoparticles confined in triphenylphosphine oxide-functionalized core-crosslinked micelles with a polyanionic shell: Synthesis, characterization, and application in aqueous biphasic hydrogenation

Core-crosslinked micelles (CCMs) with a hydrophilic polyanionic shell made of poly(sodium styrene sulfonate) chains, P(SS−Na+), a triphenylphosphine oxide-functionalized polystyrene core (TPPO@PSt) and crosslinked at the inner end of the polystyrene chains by diethylene glycol dimethacrylate (DEGDMA) were synthesized by reversible addition-fragmentation chain-transfer (RAFT) polymerization as a stable TPPO@CCM-A latex. One-pot synthesis of rhodium nanoparticles (RhNPs) by the reduction of [Rh(COD)(μ-Cl)]2 in the aqueous TPPO@CCM-A latex yielded a stable RhNP-TPPO@CCM-A latex without the need of additional stabilizer or base. This Rh-loaded latex was applied to the catalytic biphasic hydrogenation of styrene under mild conditions with complete selectivity towards ethylbenzene and corrected turnover frequencies (cTOFs) ranging from 3250 to 10,010 h−1 based on the surface atoms of the RhNPs. Importantly, the catalytic phase proved recyclable after product extraction, owing to the efficient retention of the RhNPs by the core TPPO ligands.

Development of a one-pot synthesis of rGO in water by optimizing Tour’s method parameters

Since its first synthesis in 2004, graphene has been widely studied and several different synthesis methods has been developed. Solvent exfoliation of graphite and the reduction of graphene oxide previously obtained through graphite oxidation are the most employed. In this work, we exploited synthesis conditions of a method usually employed for obtaining graphene oxide (the Tour’s method) for directly obtaining a very poorly oxidised material with characteristics like reduced graphene oxide. For the first time, a one-pot synthesis of reduced graphene oxide (rGO) is reported avoiding the use of a post-synthesis chemical or thermal reduction of the graphene oxide that requires further reagents, heat and time.

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.

One-Pot Transition-Metal-Free Synthesis of Alkynyl Amides.

Alkynyl amides play crucial roles in organic synthesis in the production of bioactive compounds and valuable heterocycles. Despite numerous studies on their synthesis, challenges persist due to the necessity of harsh or hazardous conditions and the use of costly or unstable reagents. Herein, we present a one-pot method for the synthesis of all three bonds of the alkyne under transition-metal free conditions. An important feature of this chemistry is the use of readily available feedstock chemicals, such as methyl esters and acetamides. This approach offers efficient access to a wide range of aryl and alkyl alkynyl amides and demonstrates excellent tolerance towards various functional groups in a sustainable and cost-effective manner.

Ultra-High Metal-Ions Selectivity Induced by Intramolecular Cation-π Interaction for the One-Pot Synthesis of Precise Heterometallic Architecture.

Heterometallic supramolecules, known for their unique synergistic effects, have shown broad applications in photochemistry, host-guest chemistry, and catalysis. However, there are great challenges to precisely construct heterometallic supramolecules rather than statistical mixture, due to the limited metal-ions selectivity of coordination units. Especially, heterometallic architectures precisely encoding with different metal ions usually fail to obtain in one-pot method when only one type of coordinated motif exists due to its poor metal-ion selectivity. Herein, we proposed an effective intramolecular cation-π (ICπ) strategy and successfully constructed the heterometallic supramolecule Zn2Cu4L34 by one-pot self-assembly of tritopic terpyridyl ligand L3 with Zn(II) and Cu(II), following the clear self-assembly mechanism that only thermodynamic dimers ZnL12 and Cu2L22 were constructed with model ligands L1, L2, Zn(II) and Cu(II) with perfect self-sorting and ultra-high metal-selectivity feature. The successful construction of the heterometallic supramolecule Zn2Cu4L34, encoding the definite sequence of metal ions Zn(II) and Cu(II) in one-pot method, will offer a novel approach to precisely construct heterometallic architectures.

Leveraging anchoring ligands for efficient one-pot solvothermal synthesis of PDMS functionalized iron oxide polymer nanocomposites (PNC’s)

Producing substantial quantities of high purity, narrow size distribution, magnetic polymer nanocomposites (PNC’s) has been a challenge for the nanoparticle synthesis community. In this study, we introduce a novel one-pot solvothermal synthesis technique to produce a type of PNC known as a ferrofluid. By employing a polymer (polydimethylsiloxane (PDMS)) modified with anchoring ligands as the surfactant, we eliminate the need for a post-synthesis ligand exchange, resulting in high yield and purity of the final product. This approach offers greater flexibility in polymer selection and simplifies the synthetic process. Electron microscopy, magnetic characterization, infrared spectroscopy, and thermal analysis were employed to investigate particle size, crystallinity, magnetic behavior, and surface environment. Our findings suggest that this new synthetic technique could significantly advance the development of magnetic nanoparticle-based theranostics.

Oxidative desulfurization of dibenzothiophene over V-Mo co-doped akaganeite

In this paper, V-Mo co-doped akaganeite (β-FeOOH) was prepared by one-pot hydrothermal method and the oxidative desulfurization (ODS) of dibenzothiophene over the catalyst was carefully investigated. 0.07g (ca. 0.35wt.% of model oil) of catalyst induced 100% of DBT removal in 60min with a O/S of 20:1 under 60 °C for the model oils with any of the sulfur contents, 100 ppm, 500ppm, or 1000 ppm. Moreover, the DBT removal after recycling 4 times is still 100% and it only declines to 98.04% in the fifth cycle, which indicates that the catalyst has a good stability and recycling performance. Doping V species in Mo doped β-FeOOH not only initiates a micro-variation in catalyst structure and the resultant more active •OH species but also forms a more stable structure of the catalyst, enabling the catalyst to exhibit a higher ODS reaction rate and a better reusability. The GC-MS analyses demonstrated that the DBT was converted to DBTO2 by two steps: (1) DBT→ DBTO; (2) DBTO→ DBTO2, and the former is the rate-limiting step.

One-Pot Synthesis of Propylene Carbonate through Tandem Epoxidation-Cycloaddition Reaction from Propylene and CO2

One-Pot Synthesis of Propylene Carbonate through Tandem Epoxidation-Cycloaddition Reaction from Propylene and CO₂

Green Synthesis of Magnetic Fe2O3 Nanoparticle with Chenopodium glaucum L. as Recyclable Heterogeneous Catalyst for One-Pot Reactions and Heavy Metal Adsorption

Green Synthesis of Magnetic Fe2O3 Nanoparticle with Chenopodium glaucum L. as Recyclable Heterogeneous Catalyst for One-Pot Reactions and Heavy Metal Adsorption

Stereocontrolled Hydrogenation of Conjugated Enones to Alcohols via Dual Iridium-Catalysis.

The concept of dual catalysis is an emerging area holding high potential in terms of preparative efficiency, yet faces severe challenges in compatibility of reaction conditions and interference of catalysts. The transition-metal catalyzed stereoselective hydrogenation of olefins and ketones typically proceeds under different reaction conditions and/or uses a different reductant. As a result, these two types of hydrogenations can normally not be performed in the same pot. Herein, the stereocontrolled hydrogenation of enones to saturated alcohols is described, enabled by orthogonal dual iridium catalysis, using molecular hydrogen for both reductions. In this one-pot procedure, N,P-iridium catalysts (hydrogenation active towards olefins) and NHC,P-iridium catalysts (hydrogenation active towards ketones) operated independently of one another allowing the construction of two contiguous stereogenic centers up to 99% ee, 99/1 d.r. Ultimately, by simple selection of the chirality of either ligands, the enone could be efficiently reducedto allfour stereoisomers of the saturated alcohol in equally high stereopurity. This degree of stereocontrol for the synthesis of different stereoisomers by dual transition-metal catalyzed hydrogenation was previously not attained. The generality in substituted enones (alkyl, aryl, heteroaryl) demonstrate the wide applicability of this concept.

Attapulgite-Reinforced Cellulose Hydrogels with High Conductivity and Antifreezing Property for Flexible Sensors.

Ionic conductive cellulose hydrogels are some of the most promising candidates for flexible sensors. However, it is difficult to simultaneously prepare cellulose hydrogels with high mechanical strength, good ionic conductivity, and antifreeze performance. In this work, a natural clay (attapulgite)-reinforced cellulose hydrogel was fabricated. Through a one-pot method, cellulose and attapulgite were dispersed in a concentrated ZnCl2 solution. The obtained hydrogel exhibited a dual network of hydrogen bonds and Zn2+-induced ionic interactions. Attapulgite serves as an inorganic filler that can regulate the hydrogen-bonding density among cellulose molecules and provides abundant channels for fast ion transport. By optimizing the attapulgite loading, a mechanically strong (compressive strength up to 1.10 MPa), tough (fracture energy up to 0.36 MJ m-3), highly ionic conductive (4.15 S m-1), and freezing-tolerant hydrogel was prepared. These hydrogels can be used for sensitive and stable human motion sensing, demonstrating their great potential for healthcare applications.

One-Pot Synthesis of Benzoxazoles: A Promising Approach to Aromatic Heterocyclic Compounds Preparation

One-Pot Synthesis of Benzoxazoles: A Promising Approach to Aromatic Heterocyclic Compounds Preparation