One-Pot Synthesis of Bioinspired Peptide-Decorated Apatite Nanoparticles for Nanomedicine.

Hybrid organic-inorganic bio-inspired apatite nanoparticles (NPs) are attractive for biomedical applications and especially in nanomedicine. Unfortunately, their applications in nanomedicine are limited by their broad particle size distributions and uncontrolled drug loading due to their multistep synthesis process.  Besides, very few attempts at exposing bioactive peptides on apatite NPs are made. In this work, an original one-pot synthesis of well-defined bioactive hybrid NPs composed of a mineral core of bioinspired apatite surrounded by an organic corona of bioactive peptides is reported. Dual stabilizing-bioactive agents, phosphonated polyethylene glycol-peptide conjugates, are prepared and directly used during apatite precipitation i) to form the organic corona during apatite precipitation, driving the size and shape of resulting hybrid NPs with colloidal stabilization and ii) to expose peptide moieties (RGD or YIGSR sequences) at the NPs periphery in view of conferring additional surface properties to enhance their interaction with cells. Here, the success of this approach is demonstrated, the functionalized NPs are fully characterized by Fourier-transform infrared, Raman, X-ray diffraction, solid and liquid state NMR, transmission electron microscopy, and dynamic light scattering, and their interaction with fibroblast cells is followed, unveiling a synergistic proliferative effect.

One-pot Synthesis of PdCuAg and CeO2 Nanowires Hybrid with Abundant Heterojunction Interface for Ethylene Glycol Electrooxidation.

Introducing CeO2 into Pd-based nanocatalysts for electrocatalytic reactions is a good way to solve the intermediate toxicity problem and improve the catalytic performance. Here we reported a simple strategy to synthesize the PdCuAg and CeO2 nanowires hybrid via a one-pot synthesis process under strong nanoconfined effect of specific surfactant as templates. Owing to the structural (ultrathin nanowires, abundant heterojunction/interfaces between metal and metal oxide) and compositional (Pd, Cu, Ag, CeO2) advantages, the hybrid showed significantly enhanced catalytic activity (6.06 A mgPd -1) and stability, accelerated reaction rate, and reduced activation energy toward electrocatalytic ethylene glycol oxidation reaction.

Dibenzoindolo[1,8]naphthyridines: Synthesis and Characterization of X-Shaped Aza[4,6]helicenes.

This report describes a one-pot multi-step procedure to obtain double azahelicenes via nucleophilic fluorine substitution of 2,2-di(2-bromophenyl)-1,1-difluoroalkenes and palladium-catalysed ring closing reaction. The developed synthesis approach allows easy diversification of substituents at all four fragments of the obtained X-shaped aza[4,6]helicene entity. Yields range from 20 % to 60 % among 12 product examples. X-ray single crystal analysis reveals formation of (P,P) and (M,M) enantiomer mixture of products. Optical and electrochemical properties of selected products were studied by performing UV/Vis absorption, photoluminescence and cyclic voltammetry measurements. Experimental results are supported by (TD)-DFT, NICS and NICS2BC calculations.

Preparation and characterization of bis-phosphonated polycarbohydrates.

A simple, cost-effective, one-pot method was proposed to introduce bis-phosphonic groups onto alginic acid and carboxymethyl cellulose (CMC). New derivatives were characterized by means of nuclear magnetic resonance, X-ray photoelectron, and attenuated total reflectance Fourier transform infrared spectroscopy. These analyses confirmed the successful transformation of carboxylic groups present in alginic acid and CMC into bis-phosphonic groups. Additionally, thermogravimetric analysis coupled with differential scanning calorimetry was employed to investigate the thermal properties of the bis-phosphonic derivatives of alginate and CMC. The results clearly demonstrate the char-forming ability of both studied bis-phosphonated polycarbohydrates, suggesting their potential as intumescent materials.

Design and one-pot synthesis of new substituted pyrrolo[1,2-a]thieno[3,2-e]pyrimidine as potential antitumor agents: in vitro and in vivo studies.

A new efficient and versatile one-pot three-component synthesis of substituted pyrrolo[1,2-a]thieno[3,2-e]pyrimidine derivatives has been developed. It is based on a multistep cascade reaction from 2-aminothiophenes and 2-hydroxy-4-oxobut-2-enoic acids, and derivatives of cyanoacetic acid catalyzed by diisopropylethylamine. As a result, novel pyrrolo[1,2-a]thieno[3,2-e]pyrimidine derivatives (21 compounds) were synthesized in a mild reaction conditions with a high yield. The structures of the developed compounds were confirmed by NMR and elemental analysis. The influence of electron-withdrawing or electron-donor substituents on the antitumor activity of the developed compounds has been identified. In vitro screening analysis of 21 compounds revealed six lead candidates (12aa, 12dc, 12hc, 12ic, 12lb, and 12mb) that demonstrated the most significant antitumor activity against B16-F10, 4T1 and CT26 cells. Necrosis/apoptosis assay showed that apoptosis was the predominant mechanism of cell death. Molecular docking analysis revealed several potential targets for tested compounds, i.e. phosphatidylinositol 5-phosphate 4-kinase (PI5P4K2C), proto-oncogene serine/threonine-protein kinase (Pim-1), nicotinamide phosphoribosyltransferase (NAMPT) and dihydrofolate reductase (DHFR). The lead compound (12aa) can effectively induce cell apoptosis, possesses a high yield (98 %) and requires low-cost starting chemicals for its synthesis. In vivo experiments with melanoma-bearing mice confirmed that 12aa compound resulted in the significant tumor inhibition on 15 d after the therapy. In particular, tumor volume was ∼0.19 cm3 for 50 mg/kg versus ∼2.39 cm3 in case of untreated mice and tumor weight was ∼71.6 mg for 50 mg/kg versus ∼452.4 mg when considered untreated mice. Thus, our results demonstrated the high potential of the 12aa compound in the treatment of melanoma and can be recommended for further preclinical studies.

Design, spectroscopic characterizations, and biological investigation of oxospiro[chromine-4,3-indolene]-based compounds as promising antiproliferative EGFR inhibitors and antimicrobial agents.

Utilizing microwave heating and an aqueous saturated solution of K2CO3 as a catalyst, a rapidone-pot synthesis of oxospiro[chromene-4.3-indoline] derivatives was produced in high yields. The experimental results confirmed that the saturated solution of K2CO3 gives outstanding yield to dangerous metals and strong bases during investigations into high-performance catalysts. The used catalyst is green, affordable, incredibly mild, and widely accessible. However, it generates samples, reduces the amount of byproducts, and is expected to be used in industrial-scale heterocyclic derivatives. New oxospiro[chromene-4.3-indoline] derivatives have been created from various isatin by condensing with various phenols. The biological activities results showed that when compared to erlotinib, the derivatives 3b, 4b, 5b, and 6b were the most effective analogues on A549, MCF-7, HepG-2, and HCT-116 cells, with an IC50 range of 3.32 to 11.88 µM. In A549 cells, compounds 3b, 4b, 5b, and 6b induced apoptosis, as shown by the up-regulation of Bax, the up-regulation of Bcl-2, and the stimulation of caspase-3 and -9. With IC50 value of 0.19 ± 0.09, compound3b was demonstrated to be the most effective against EGFRWT. Compounds 4b and 6b have good antibacterial activity toward Staphylococcus aureus, comparable to ciprofloxacin, and about half as much activity as ampicillin, according to the MIC value. Compound 6b's MIC is about 25% lower than clotrimazole drug. The in silico molecular docking outcomes of compounds 3b, 4b, 5b, and 6b in the EGFR active site depicted their ability to adopt essential binding interactions compared to the reference Erlotinib. Moreover, the investigation of the physicochemical properties of the most promising dual acting antiproliferative and antimicrobial compounds 4b and 6b through the egg-boiled method illustrated acceptable lipophilicity, GIT absorption, and blood-brain barrier penetration characteristics.

Development of a "turn off" fluorescent molecularly imprinted nanoparticle-based sensor for selective captopril quantification in synthetic urine and wastewater samples.

The combination of silica nanoparticles with fluorescent molecularly imprinted polymers (Si-FMIPs) prepared by a one-pot sol-gel synthesis method to act as chemical sensors for the selective and sensitive determination of captopril is described. Several analytical parameters were optimized, including reagent ratio, solvent, concentration of Si-FMIP solutions, and contact time. Fourier-transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), and the ninhydrin assay were used for characterization. The selectivity was evaluated against molecules belonging to other drug classes, such as fluoroquinolones, nonacid nonopioids, benzothiadiazine, alpha amino acids, and nitroimidazoles. Under optimized conditions, the Si-FMIP-based sensor exhibited a working range of 1-15 µM, with a limit of detection (LOD) of 0.7 µM, repeatability of 6.4% (n = 10), and suitable recovery values at three concentration levels (98.5% (1.5 µM), 99.9% (3.5 µM), and 99.2% (7.5 µM)) for wastewater samples. The sensor provided a working range of 0.5-15 µM for synthetic urine samples, with an LOD of 0.4 µM and a repeatability of 7.4% (n = 10) and recovery values of 93.7%, 92.9%, and 98.0% for 1.0 µM, 3.5 µM, and 10 µM, respectively. In conclusion, our single-vessel synthesis approach for Si-FMIPs proved to be highly effective for the selective determination of captopril in wastewater and synthetic urine samples.

Helical Nanofiber Photoelectric Synaptic Devices for an Artificial Vision Nervous System.

Inspired by the helical structure and the resultant exquisite functions of biomolecules, helical polymers have received increasing attention. Here, a series of poly(3-hexylthiophene)-block-poly(phenyl isocyanide) (P3HT-b-PPI) copolymers were prepared using a simple one-pot living polymerization method. Interestingly, the P3HT80-b-PPI30 films were found to have a helical nanofiber structure. The corresponding device has superior optoelectronic properties, such as a broadened spectral response range from the visible band to the deep ultraviolet (DUV) and an approximately 5-fold longer carrier decay time after DUV light stimulation. An energy consumption of 1.44 fJ per synaptic event was obtained, which is the lowest energy consumption achieved so far with DUV light stimulation. The encryption and decryption of images are implemented using an array of devices. Finally, a photoreceptor neural pathway was constructed to achieve early warning for the recognition of the display of harmful light. This research provides an effective strategy for the development of a novel optoelectronic synaptic device.

One-Pot Synthesis and Surfactant Removal from MCM-41 Using Microwave Irradiation.

This research pioneers the application of microwave irradiation as an innovative strategy for one-pot synthesis and surfactant elimination (cetyltrimethylammonium bromide-CTAB) from MCM-41, introducing a rapid and efficient methodology. MCM-41 silica is widely utilized in various applications due to its unique textural and structural properties. Nonetheless, the presence of residual surfactants after synthesis poses a challenge to its effective application. MCM-41 synthesis, conducted in a microwave reactor at 60 °C, provided a result within 0.5 to 1 h. Comprehensive analyses of structural, chemical, morphological, and surface characteristics were undertaken, with a focus on the impact of synthesis time on these properties. Surfactant extraction involved the use of ethanol as a solvent at 120 °C for 6 min within the microwave reactor. The acquired particles, coupled with the properties of textural and structural features, affirmed the efficacy of the synthesis process, resulting in the synthesis of MCM-41 within 36 min. This study presents the first instance of one-pot synthesis and surfactant removal from MCM-41 using a microwave reactor. The proposed method not only addresses the surfactant removal challenge, but also substantially accelerates the synthesis process, thereby enhancing the potential for MCM-41's application in diverse fields.

One-Pot Cu/SAPO-34 for Continuous Methane Selective Oxidation to Methanol.

Cu/SAPO-34 synthesized via a one-pot method with relatively low silicon content and copper loading at around 2 wt.% facilitated continuous oxidation of methane to methanol with a methanol space time yield of 504 µmolCH3OH/gcat/h. Remarkably, the methanol yield exceeded 1800 mmolCH3OH/molCu/h at 623 K. Typically, the presence of trace oxygen in the system was the key to maintaining the high selectivity to methanol. Characterization results from a series of techniques, including XRD, SEM, TEM, H2-TPR, NH3-TPD, UV-vis, and FTIR, indicated that Cu2+ existed in the position where it moves from hexagonal rings to elliptical cages as the active center.

One-pot synthesis of N-doped petroleum coke-based microporous carbon for high-performance CO2 adsorption and supercapacitors.

Waste resource utilization of petroleum coke is crucial for achieving global carbon emission reduction. Herein, a series of N-doped microporous carbons were fabricated from petroleum coke using a one-pot synthesis method. The as-prepared samples had a large specific surface area (up to 2512 m2/g), a moderate-high N content (up to 4.82 at.%), and high population (55%) of ultra-micropores (<0.7 nm). Regulating the N content and ultra-microporosity led to efficient CO2 adsorption and separation. At ambient pressure, the optimal N-doped petroleum coke-based microporous carbon exhibited the highest CO2 uptake of 4.25 mmol/g at 25°C and 6.57 mmol/g at 0°C. These values are comparable or even better than those of numerous previously reported adsorbents prepared by multistep synthesis, primarily due to the existence of ultra-micropores. The sample exhibited excellent CO2/N2 selectivity at 25°C owing to the abundant basic pyridinic and pyrrolic N species; and showed superior CO2 adsorption-desorption cycling performance, which was maintained at 97% after 10 cycles at 25°C. Moreover, petroleum coke-based microporous carbon, with a considerably high specific surface area and hierarchical pore structure, exhibited excellent electrochemical performance over the N-doped sample, maintaining a favorable specific capacitance of 233.25 F/g at 0.5 A/g in 6 mol/L KOH aqueous electrolyte. This study provides insight into the influence of N-doping on the porous properties of petroleum coke-based carbon. Furthermore, the as-prepared carbons were found to be promising adsorbents for CO2 adsorption, CO2/N2 separation and electrochemical application.

Facile Synthesis of Anhydrous Rare-Earth Trichlorides from their Oxides in Chloridoaluminate Ionic Liquids.

Wide applications of anhydrous rare-earth (RE) trichlorides RECl3 in organometallic chemistry, for the synthesis of optical and magnetic materials, and as catalysts require a facile approach for their synthesis. The known methods use or produce toxic substances, are complicated and have limited reliability and upscaling. It has been shown that task-specific ionic liquids (ILs) can dissolve many metal oxides without special reaction conditions at moderate temperature, making the metals accessible to downstream chemistry. Using imidazolium chloridoaluminate ILs, pure crystalline anhydrous RECl3 (RE=La-Nd, Sm-Dy) can be synthesized in one step from RE oxides in high yield. The Lewis acidic IL acts as solvent and reaction partner. The by-product [Al4 O2 Cl10 ]2- , which was detected spectroscopically, remains in solution. The reacted IL can be removed quantitatively by washing. ILs with various imidazolium cations and AlCl3 content and the effect of temperature and reaction time were tested.

Merging High-Pressure Syngas Metal Catalysis and Biocatalysis in Tandem One-Pot Processes for the Synthesis of Nonchiral and Chiral Alcohols from Alkenes in Water.

While simultaneously proceeding reactions are among the most fascinating features of biosynthesis, this concept of tandem processes also offers high potential in the chemical industry in terms of less waste production and improved process efficiency and sustainability. Although examples of one-pot chemoenzymatic syntheses exist, the combination of completely different reaction types is rare. Herein, we demonstrate that extreme "antipodes" of the "worlds of catalysis", such as syngas-based high-pressure hydroformylation and biocatalyzed reduction, can be combined within a tandem-type one-pot process in water. No significant deactivation was found for either the biocatalyst or the chemocatalyst. A proof-of-concept for the one-pot process starting from 1-octene was established with >99 % conversion and 80 % isolated yield of the desired alcohol isomers. All necessary components for hydroformylation and biocatalysis were added to the reactor from the beginning. This concept has been extended to the enantioselective synthesis of chiral products by conducting the hydroformylation of styrene and an enzymatic dynamic kinetic resolution in a tandem mode, leading to an excellent conversion of >99 % and an enantiomeric ratio of 91 : 9 for (S)-2-phenylpropanol. The overall process runs in water under mild and energy-saving conditions, without any need for intermediate isolation.

Structural Design Induced Electronic Optimization in Single-Phase MoCoP Nanocrystal for Boosting Oxygen Reduction, Oxygen Evolution, and Hydrogen Evolution.

Structural and compositional design of multifunctional materials is critical for electrocatalysis, but their rational modulation and effective synthesis remain a challenge. Herein, a controllable one-pot synthesis for construction of trifunctional sites and preparation of porous structures is adopted for synthesizing dispersed MoCoP sites on N, P codoped carbonized substance. This tunable synthetic strategy also endorses the exploration of the electrochemical activities of Mo (Co)-based unitary, Mo/Co-based dual and MoCo-based binary metallic sites. Eventually benefiting from the structural regulation, MoCoP-NPC shows excellent oxygen reduction abilities with a half-wave potential of 0.880 V, and outstanding oxygen evolution and hydrogen evolution performance with an overpotential of 316 mV and 91 mV, respectively. MoCoP-NPC-based Zn-air battery achieves excellent cycle stability for 300 h and a high open-circuit voltage of 1.50 V. When assembled in a water-splitting device, MoCoP-NPC reaches 10 mA cm-2 at 1.65 V. Theoretical calculations demonstrate that the Co atom in the single-phase MoCoP has a low energy barrier for oxygen evolution reaction (OER) owing to the migration of Co 3d orbital toward the Fermi level. This work shows a simplified method for controllable preparation of prominent trifunctional catalysts.

Chemoenzymatic Synthesis of Sterically Hindered Biaryls by Suzuki Coupling and Vanadium Chloroperoxidase Catalyzed Halogenations.

Halogenated biaryls are vital structural skeletons in bioactive products. In this study, an effective chemoenzymatic halogenation by vanadium-dependent chloroperoxidase from Camponotus inaequalis (CiVCPO) enabled the transformation of freely rotating biaryl bonds to sterically hindered axis. The yields were up to 84 % for the tribrominated biaryl products and up to 65 % when isolated. Furthermore, a one-pot, two-step chemoenzymatic strategy by incorporating transition metal catalyzed Suzuki coupling and the chemoenzymatic halogenation in aqueous phase were described. This strategy demonstrates a simplified one-pot reaction sequence with organometallic and biocatalytic procedures under economical and environmentally beneficial conditions that may inspire further research on synthesis of sterically hindered biaryls.

One-Pot Tandem Coupling Method for the Short-Step Formal Synthesis of Riccardin C.

One-pot reactions reduce reagent amounts and circumvent process treatments, such as work-up and purifications in multi-step reactions. In this study, we achieved the formal total synthesis of riccardin C through a one-pot reaction by simultaneously linking four units through two Sonogashira coupling reactions and one Suzuki coupling reaction, followed by reduction and deprotection. Thus, this one-pot method comprised five steps and did not require the purification of intermediate reaction mixtures, which saves resources, such as reagents and solvents, and expedites the work process.

One-pot Synthesis of Phosphorus-modified ZSM-5 Zeolite by Solid-state Method and its MTO Catalytic Performance.

The traditional hydrothermal synthesis strategy of ZSM-5 zeolite is energy-consumption accompanying by pollution issues. Herein, phosphorus-modified layered ZSM-5 zeolites (PZ) were obtained by one-pot synthesis under solvent-free conditions. The synthesized samples were fully characterized by XRD, SEM, BET, NH3 -TPD and FTIR. The effect of phosphorus addition on the morphology and catalytic activity of ZSM-5 was investigated. The results showed that phosphorus-modified ZSM-5 zeolites exhibited higher light olefin (ethylene and propylene) selectivity (above 50 %) and longer catalytic lifetime (33 h) in methanol to olefin (MTO) reaction when the weight hourly space velocity was 4 h-1 . Phosphorus-modified ZSM-5 zeolite synthesized by in situ solvent-free method, which not only reduced the discharge of sewage but also showed a simple method to realize the introduction of phosphorous species, which provided a new idea for phosphorus modification of ZSM-5 zeolite.

One-Pot Synthesis of Chiral 1-Aryl-2-Aminoethanols via Ir-Catalyzed Asymmetric Hydrogenation.

A straightforward synthesis approach to chiral 1-aryl-2-aminoethanols via the one-pot asymmetric hydrogenation catalyzed by Ir catalyst was developed. This tandem process involves the in situ generation of α-amino ketones via the nucleophilic substitution of α-bromoketones with amines and the Ir-catalyzed asymmetric hydrogenation of ketone intermediates to provide diverse enantiomerically enriched ß-amino alcohols. The excellent yields and enantioselectivities (up to 96 % yield and up to >99 % ee) with a wide substrate scope in this one-pot strategy were obtained.

Mechanochemical Solvent-Free One-Pot Synthesis of Poly-Functionalized 5-(Arylselanyl)-1H-1,2,3-triazoles Through a Copper(I)-Catalyzed Click Reaction.

A mechanochemistry-driven practical and efficient synthetic protocol for accessing diverse series of biologically relevant poly-functionalized 5-(arylselanyl)-1H-1,2,3-triazoles through copper(I)-catalyzed click reaction between aryl/heteroaryl acetylenes, diaryl diselenides, benzyl bromides, and sodium azide has been accomplished under high-speed ball-milling. Advantages of this method include operational simplicity, avoidance of using solvent and external heating, one-pot synthesis, short reaction time in minutes, good to excellent yields, broad substrate scope, and gram-scale applications. Furthermore, synthesized organoselenium compounds were synthetically diversified to biologically promising selenones.

Towards Alzheimer's disease-related targets: One-pot Cu(I)- mediated synthesis of new nitroindazolyltriazoles.

In this work, we have investigated the one pot strategy for the Cu(I)-mediated synthesis of new triazoles bearing nitroindazole moieties using different copper catalysts. The biological activity of newly synthesized nitroindazolyltriazoles towards Alzheimer's disease-related targets, namely cholinesterases, monoamine oxidases, and amyloid aggregation, were investigated. Predictions of target affinity, physicochemical parameters, gastrointestinal absorption and brain penetration were achieved by means of in silico tools.