Browse
Submit Data
Databases
API
Help

Dataset Information

23 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

In Situ Anodically Oxidized BMIm-BF₄: A Safe and Recyclable BF₃ Source.

ABSTRACT: The anodic oxidation of 1-butyl-3-methylimidazolium tetrafluoroborate (BMIm-BF₄) efficiently generates BF₃ from BF₄^-. This Lewis acid, strongly bound to the ionic liquids, can be efficiently used in classical BF₃-catalyzed reactions. We demonstrated the BF₃/BMIm-BF₄ reactivity in four reactions, namely, a domino Friedel-Crafts/lactonization of phenols, the Povarov reaction, the Friedel-Crafts benzylation of anisole, and the multicomponent synthesis of tetrahydro-11H-benzo[a]xanthen-11-ones. In comparison with literature data using BF₃-Et₂O in organic solvents, in all the presented cases, analogous or improved results were obtained. Moreover, the noteworthy advantages of the developed method are the in situ generation of BF₃ (no storing necessity) in the required amount, using only the electron as redox reagent, and the recycling of BMIm-BF₄ for multiple subsequent runs.

SUBMITTER: Bortolami M

PROVIDER: S-EPMC8609525 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Integrating Molecular Simulations with Machine Learning Guides in the Design and Synthesis of [BMIM][BF4]/MOF Composites for CO2/N2 Separation.

Project description:Considering the existence of a large number and variety of metal-organic frameworks (MOFs) and ionic liquids (ILs), assessing the gas separation potential of all possible IL/MOF composites by purely experimental methods is not practical. In this work, we combined molecular simulations and machine learning (ML) algorithms to computationally design an IL/MOF composite. Molecular simulations were first performed to screen approximately 1000 different composites of 1-n-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF4]) with a large variety of MOFs for CO2 and N2 adsorption. The results of simulations were used to develop ML models that can accurately predict the adsorption and separation performances of [BMIM][BF4]/MOF composites. The most important features that affect the CO2/N2 selectivity of composites were extracted from ML and utilized to computationally generate an IL/MOF composite, [BMIM][BF4]/UiO-66, which was not present in the original material data set. This composite was finally synthesized, characterized, and tested for CO2/N2 separation. Experimentally measured CO2/N2 selectivity of the [BMIM][BF4]/UiO-66 composite matched well with the selectivity predicted by the ML model, and it was found to be comparable, if not higher than that of all previously synthesized [BMIM][BF4]/MOF composites reported in the literature. Our proposed approach of combining molecular simulations with ML models will be highly useful to accurately predict the CO2/N2 separation performances of any [BMIM][BF4]/MOF composite within seconds compared to the extensive time and effort requirements of purely experimental methods.

| S-EPMC10080536 | biostudies-literature

Catalytic asymmetric nucleophilic fluorination using BF3·Et2O as fluorine source and activating reagent.

Project description:Fluorination using chiral catalytic methods could result in a direct access to asymmetric fluorine chemistry. However, challenges in catalytic asymmetric fluorinations, especially the longstanding stereochemical challenges existed in BF3·Et2O-based fluorinations, have not yet been addressed. Here we report the catalytic asymmetric nucleophilic fluorination using BF3·Et2O as the fluorine reagent in the presence of chiral iodine catalyst. Various chiral fluorinated oxazine products were obtained with good to excellent enantioselectivities (up to >99% ee) and diastereoselectivities (up to >20:1 dr). Control experiments (the desired fluoro-oxazines could not be obtained when Py·HF or Et3N·3HF were employed as the fluorine source) indicated that BF3·Et2O acted not only as a fluorine reagent but also as the activating reagent for activation of iodosylbenzene.

| S-EPMC8233348 | biostudies-literature

Magnetic recyclable CoFe2O4@PPy prepared by in situ Fenton oxidization polymerization with advanced photo-Fenton performance.

Project description:Here we present a magnetic recyclable photo-Fenton catalyst CoFe2O4@PPy with uniform morphology and excellent dispersibility prepared via simple in situ Fenton oxidization polymerization. The CoFe2O4 core provides good magnetic recyclability for the catalysts as well as the ion source for catalyzed decomposition of H2O2 in PPy coating. The optimal catalytic effect can be obtained by adjusting the ratio of CoFe2O4 and PPy. Methylene blue, Methyl orange and Rhodamine B (RhB) employed as model pollutants certificated that the catalyst exhibits a wide range of photodegradability. The decoloration rates reach nearly 100% in the photodegradation of 10 mg L-1 RhB after 2 h visible-light irradiation and only low toxicity small molecules are detected by LC-MS. Moreover, the catalytic activity remains after 5 cycles with decoloration rates up to 90%. The degradation measurement in the presence of scavengers of reactive species reveals that the positive holes (h+) and hydroxyl radical (·OH) are the main reactive oxygen species in the CoFe2O4@PPy system. The performance enhancement may be attributed to the combination of improved Fenton activity by coordinated Fe2+ and PPy redox pairs and photo-catalytic activity by broaden adsorption and photo-generated charge separation.

| S-EPMC9048221 | biostudies-literature

In Situ Synthesis of Ag-Fe3O4 Nanoparticles Immobilized on Pure Cellulose Microspheres as Recyclable and Biodegradable Catalysts.

Project description:The preparation of reusable and eco-friendly materials from renewable biomass resources such as cellulose is an inevitable choice for sustainable development. In this work, cellulose was dissolved in 7 wt % NaOH/12 wt % urea aqueous solution at -12 °C with rapid stirring. Cellulose microspheres (Cels) were fabricated by a sol-gel transition method. Subsequently, novel magnetic Ag-Fe3O4 nanoparticles (NPs) supported on cellulose microspheres were successfully constructed by an in situ one-pot synthesis. The magnetic cellulose microspheres (MCels) displayed a spherical shape with mesoporous structure and had a narrow particle size distribution (10-20 ?m). Many nanopores with a pore diameter of 5-40 nm were observed in MCels. The Ag-Fe3O4 NPs were immobilized by anchoring with the hydroxyl groups on the surface of Cels. MCels were applied as a microreactor to evaluate their catalytic activities. 4-Nitrophenol (4-NP) could be reduced to 4-aminophenol (4-AP) in 5 min, catalyzed by MCels. Moreover, the magnetic microspheres exhibited a small hysteresis loop and low coercivity. Thus, MCels could be quickly gathered in water under a magnetic field in 10 s, as well as almost 9 cycle times, maintaining relatively high catalytic activity. In this work, cellulose matrix as the catalyst support could be biodegraded completely in the environment. It provided a green process for the utilization of biomass in nanocatalytic applications.

| S-EPMC7178767 | biostudies-literature

In situ oxidized TiO2/MXene ultrafiltration membrane with photocatalytic self-cleaning and antibacterial properties.

Project description:Self-cleaning, antimicrobial ultrafiltration membranes are urgently needed to alleviate the low flux problems caused by membrane fouling in water treatment processes. In this study, in situ generated nano-TiO2 MXene lamellar materials were synthesized and then 2D membranes were fabricated using vacuum filtration. The presence of nano TiO2 particles as an interlayer support layer widened the interlayer channels, and also improved the membrane permeability. The TiO2/MXene composite on the surface also showed an excellent photocatalytic property, resulting in enhanced self-cleaning properties and improved long-term membrane operational stability. The best overall performance of the TiO2/MXene membrane at 0.24 mg cm-2 loading was optimal, with 87.9% retention and 211.5 L m-2 h-1 bar-1 flux at a filtration of 1.0 g L-1 bovine serum albumin solution. Noticeably, the TiO2/MXene membranes showed a very high flux recovery under UV irradiation with a flux recovery ratio (FRR) of 80% as compared to the non-photocatalytic MXene membranes. Moreover, the TiO2/MXene membranes demonstrated over 95% resistance against E. coli. And the XDLVO theory also showed that the loading of TiO2/MXene slowed down the fouling of the membrane surface by protein-based contaminants.

| S-EPMC10209591 | biostudies-literature

BF2-Azadipyrromethene Fluorophores for Intraoperative Vital Structure Identification.

Project description:A series of mono- and bis-polyethylene glycol (PEG)-substituted BF2-azadipyrromethene fluorophores have been synthesized with emissions in the near-infrared region (700-800 nm) for the purpose of fluorescence guided intraoperative imaging; chiefly ureter imaging. The Bis-PEGylation of fluorophores resulted in higher aqueous fluorescence quantum yields, with PEG chain lengths of 2.9 to 4.6 kDa being optimal. Fluorescence ureter identification was possible in a rodent model with the preference for renal excretion notable through comparative fluorescence intensities from the ureters, kidneys and liver. Ureteral identification was also successfully performed in a larger animal porcine model under abdominal surgical conditions. Three tested doses of 0.5, 0.25 and 0.1 mg/kg all successfully identified fluorescent ureters within 20 min of administration which was sustained up to 120 min. 3-D emission heat map imaging allowed the spatial and temporal changes in intensity due to the distinctive peristaltic waves of urine being transferred from the kidneys to the bladder to be identified. As the emission of these fluorophores could be spectrally distinguished from the clinically-used perfusion dye indocyanine green, it is envisaged that their combined use could be a step towards intraoperative colour coding of different tissues.

| S-EPMC10004488 | biostudies-literature

In situ transport measurements reveal source of mobility enhancement of MoS2 and MoTe2 during dielectric deposition.

Project description:Layered transition metal dichalcogenides (TMDs) and other two-dimensional (2D) materials are promising candidates for enhancing the capabilities of complementary metal-oxide-semiconductor (CMOS) technology. Field-effect transistors (FETs) made with 2D materials often exhibit mobilities below their theoretical limit, and strategies such as encapsulation with dielectrics grown by atomic layer deposition (ALD) have been explored to tune carrier concentration and improve mobility. While molecular adsorbates are known to dope 2D materials and influence charge scattering mechanisms, it is not well understood how ALD reactants affect 2D transistors during growth, motivating in situ or operando studies. Here, we report electrical characterization of MoS2 and MoTe2 FETs during ALD of MoOx. The field effect mobility improves significantly within the first five cycles of ALD growth using Mo(NMe2)4 as the metal-organic precursor and H2O as the oxidant. Analyses of the in situ transconductance at the growth temperature and ex situ variable temperature transconductance measurements indicate that the majority of the mobility enhancement observed at the beginning of dielectric growth is due to screening of charged impurity scattering by the adlayer. Control experiments show that exposure to only H2O or O2 induces more modest and reversible electronic changes in MoTe2 FETs, indicating that negligible oxidation of the TMD takes place during the ALD process. Due to the strong influence of the first <2 nm of deposition, when the dielectric adlayer may be discontinuous and still evolving in stoichiometry, this work highlights the need for further assessment of nucleation layers and initial deposition chemistry, which may be more important than the bulk composition of the oxide itself in optimizing performance and reproducibility.

| S-EPMC7727257 | biostudies-literature

Oxidized konjac glucomannan: A safe dietary fiber influencing mouse gut microbiota.

Project description:In this 13-week study, the potential effects of oxidized konjac glucomannan (OKGM) on ICR mice's metabolic health and gut microbiota were investigated and contrasted with enzyme-hydrolyzed KGM (EKGM) at a same molecular weight. Mice were fed diets containing 0 %, 2.5 %, 5.0 %, and 7.5 % of OKGM for 13 weeks. Results indicated that OKGM induced no adverse effects, with overall health, body weight gain, food consumption, and clinical pathology parameters being comparable to the control group. The no-observed-adverse-effect-level for OKGM was determined at 7.5 % in the diet, corresponding to 10.21 and 12.01 g/kg/day for male and female mice, respectively. OKGM intake positively regulated gut microbiota, characterized by a reduction in the relative abundance of Firmicutes, an increase in Bacteroidetes, and an enhanced presence of Lactobacillus, particularly Lactobacillus reuteri. In comparison, EKGM differently modulated the microbiota, notably increasing Muribaculaceae. These findings suggest that OKGM has the potential to be a functional food additive.

| S-EPMC10801215 | biostudies-literature

Chemically recyclable polyesters from CO2, H2, and 1,3-butadiene.

Project description:Chemically recyclable solid polymeric materials with commercializable properties only using CO2 and inexpensive bulk chemicals as chemical feedstock can open a brand-new avenue to economically viable, large-scale fixation of CO2 over a long period of time. Despite previous great advancements, development of such a kind of CO2-based polymers remains a long-term unsolved research challenge of great significance. Herein, we reported the first methodology to polymerize six-membered lactone with two substituents vicinal to the ester group (HL), a compound previously found to be non-polymerizable. The present methodology enables the first synthesis of chemically recyclable solid polyesters (polyHL) with a high CO2 content (28 wt %) and large molecular weights (M n up to 613.8 kg mol-1). Transparent membranes with promising pressure-sensitive adhesive (PSA) properties comparable with their commercial counterparts can be conveniently fabricated from the polyesters. Mechanistic studies indicate that rigorous removal of water impurity is the key to the successful polymerization of the relatively inert disubstituted six-membered lactone. A complete monomer recovery from polyHL was also successfully achieved under mild catalytic conditions. The synthesis of polyHL only requires CO2 and two inexpensive bulk chemicals, H2 and 1,3-butadiene, as the starting materials, thus providing a new strategy for potential scalable chemical utilization of CO2 with desirable economic values and concomitant mitigation of CO2 emissions. This work should inspire future research to make useful new solid CO2-based polymers that can meaningfully increase the scale of chemical utilization of CO2 and promote the contribution of chemical utilization of CO2 to global mitigation of CO2 emissions.

| S-EPMC8881707 | biostudies-literature

Selective Late-Stage Sulfonyl Chloride Formation from Sulfonamides Enabled by Pyry-BF4.

Project description:Reported here is a simple and practical functionalization of primary sulfonamides, by means of a pyrylium salt (Pyry-BF4 ), with nucleophiles. This simple reagent activates the poorly nucleophilic NH2 group in a sulfonamide, enabling the formation of one of the best electrophiles in organic synthesis: a sulfonyl chloride. Because of the variety of primary sulfonamides in pharmaceutical contexts, special attention has been focused on the direct conversion of densely functionalized primary sulfonamides by a late-stage formation of the corresponding sulfonyl chloride. A variety of nucleophiles could be engaged in this transformation, thus permitting the synthesis of complex sulfonamides, sulfonates, sulfides, sulfonyl fluorides, and sulfonic acids. The mild reaction conditions and the high selectivity of Pyry-BF4 towards NH2 groups permit the formation of sulfonyl chlorides in a late-stage fashion, tolerating a preponderance of sensitive functionalities.

| S-EPMC6916363 | biostudies-literature