Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Au3+/Au⁰ Supported on Chromium(III) Terephthalate Metal Organic Framework (MIL-101) as an Efficient Heterogeneous Catalystfor Three-Component Coupling Synthesis of Propargylamines.

ABSTRACT: Post-synthesis modification is a useful method for the functionalization of metal-organic frameworks (MOFs). A novel catalyst Au@MIL-101-ED-SA (ED = ethylenediamine, SA = salicylaldehyde), containing coexisting Au3+ ions and Au⁰ nanoparticles, was prepared successfully by post-synthesis modification with ethylenediamine, salicylaldehyde and gold. Gold nanoparticles supported on MIL-101 (Au@MIL-101) were prepared successfully by the impregnation method. Au@MIL-101-ED-SA and Au@MIL-101 were characterized by N₂ adsorption-desorption, X-ray diffraction, infrared spectroscopy, thermogravimetric analysis, X-ray photoelectron spectroscopy, and inductively coupled plasma-optical emission spectrometry. Au@MIL-101-ED-SA and Au@MIL-101 were applied as environmentally friendly catalysts in the three-component coupling reaction of aldehydes, amines, and alkynes for the preparation of diverse propargylamines. Au@MIL-101-ED-SA contained a fraction of cationic gold (Au3+/Au⁰ = 0.9) and showed higher catalytic activity than Au@MIL-101, which was prepared by the impregnation method. Furthermore, the reactions were performed under heterogeneous conditions and the novel catalyst was successfully recycled for four consecutive runs.

SUBMITTER: Liu L

PROVIDER: S-EPMC5459189 | biostudies-other | 2017 Jan

REPOSITORIES: biostudies-other

ACCESS DATA

Json Xml

Similar Datasets

Metal-Organic Framework MIL-101(Cr) as an Efficient Heterogeneous Catalyst for Clean Synthesis of Benzoazoles.

Project description:A metal-organic framework [MIL-101(Cr)] was used as an efficient heterogeneous catalyst in the synthesis of benzoazoles (benzimidazole, benzothiazole, and benzoxazole), and quantitative conversion of products were obtained under optimized reaction conditions. The catalyst could be simply extracted from the reaction mixture, providing an efficient and clean synthetic methodology for the synthesis of benzoazoles. The MIL-101(Cr) catalyst could be reused without a remarkable decrease in its catalytic efficiency.

| S-EPMC6643801 | biostudies-literature

Molecular promoting of aluminum metal-organic framework topology MIL-101 by N,N-dimethylformamide.

Project description:In situ NMR and DFT modeling demonstrate that N,N-dimethylformamide (DMF) promotes the formation of metal-organic framework NH2-MIL-101(Al). In situ NMR studies show that upon dissociation of an aluminum-coordinated aqua ligand in NH2-MOF-235(Al), DMF forms a H-Cl-DMF complex during synthesis. This reaction induces a transformation from the MOF-235 topology into the MIL-101 topology. Electronic structure density functional theory (DFT) calculations show that the use of DMF instead of water as the synthesis solvent decreases the energy gap between the kinetically favored MIL-101 and thermodynamically favored MIL-53 products. DMF therefore promotes MIL-101 topology both kinetically and thermodynamically.

| S-EPMC4051174 | biostudies-literature

A Bimetallic Organic Framework with Mn in MIL-101(Cr) for Lithium-Sulfur Batteries.

Project description:Lithium-sulfur batteries (LSBs) show excellent performance in terms of specific capacity and energy density. However, the cyclic stability of LSBs is compromised due to the "shuttle effect", which hinders the practical applications of LSBs. Herein, a metal-organic framework (MOF) based on Cr ions as the main body composition, commonly known as MIL-101(Cr), was utilized to minimize the shuttle effect and improve the cyclic performance of LSBs. To obtain MOFs with a certain adsorption capacity for lithium polysulfide and a certain catalytic capacity, we propose an effective strategy of incorporating sulfur-loving metal ions (Mn) into the skeleton to enhance the reaction kinetics at the electrode. Based on the oxidation doping method, Mn2+ was uniformly dispersed in MIL-101(Cr) to produce bimetallic Cr2O3/MnOx as a novel sulfur-carrying cathode material. Then, a sulfur injection process was carried out by melt diffusion to obtain the sulfur-containing Cr2O3/MnOx-S electrode. Moreover, an LSB assembled with Cr2O3/MnOx-S showed improved first-cycle discharge (1285 mAh·g-1 at 0.1 C) and cyclic performance (721 mAh·g-1 at 0.1 C after 100 cycles), and the overall performance was much better than that of monometallic MIL-101(Cr) as a sulfur carrier. These results revealed that the physical immobilization method of MIL-101(Cr) positively affected the adsorption of polysulfides, while the bimetallic composite Cr2O3/MnOx formed by the doping of sulfur-loving Mn2+ into the porous MOF produced a good catalytic effect during LSB charging. This research provides a novel approach for preparing efficient sulfur-containing materials for LSBs.

| S-EPMC10223926 | biostudies-literature

Bimetallic Au-Pd alloy nanoparticles supported on MIL-101(Cr) as highly efficient catalysts for selective hydrogenation of 1,3-butadiene.

Project description:Gold-palladium (Au-Pd) bimetallic nanoparticle (NP) catalysts supported on MIL-101(Cr) with Au : Pd mole ratios ranging from 1 : 3 to 3 : 1 were prepared through coimpregnation and H2 reduction. Au-Pd NPs were homogeneously distributed on the MIL-101(Cr) with mean particle sizes of 5.6 nm. EDS and XPS analyses showed that bimetallic Au-Pd alloys were formed in the Au(2)Pd(1)/MIL-101(Cr). The catalytic performance of the catalysts was explored in the selective 1,3-butadiene hydrogenation at 30-80 °C on a continuous fixed bed flow quartz reactor. The bimetallic Au-Pd alloy particles stabilized by MIL-101(Cr) presented improved catalytic performance. The as-synthesized bimetallic Au(2)Pd(1)/MIL-101(Cr) with 2 : 1 Au : Pd mole ratio showed the best balance between the activity and butene selectivity in the selective 1,3-butadiene hydrogenation. The Au-Pd bimetallic-supported catalysts can be reused in at least three runs. The work affords a reference on the utilization of a MOF and alloy nanoparticles to develop high-efficiency catalysts.

| S-EPMC9056711 | biostudies-literature

Glucose recovery from aqueous solutions by adsorption in metal-organic framework MIL-101: a molecular simulation study.

Project description:A molecular simulation study is reported on glucose recovery from aqueous solutions by adsorption in metal-organic framework MIL-101. The F atom of MIL-101 is identified to be the most favorable adsorption site. Among three MIL-101-X (X = H, NH2 or CH3), the parent MIL-101 exhibits the highest adsorption capacity and recovery efficacy. Upon functionalization by -NH2 or -CH3 group, the steric hindrance in MIL-101 increases; consequently, the interactions between glucose and framework become less attractive, thus reducing the capacity and mobility of glucose. The presence of ionic liquid, 1-ethyl-3-methyl-imidazolium acetate, as an impurity reduces the strength of hydrogen-bonding between glucose and MIL-101, and leads to lower capacity and mobility. Upon adding anti-solvent (ethanol or acetone), a similar adverse effect is observed. The simulation study provides useful structural and dynamic properties of glucose in MIL-101, and it suggests that MIL-101 might be a potential candidate for glucose recovery.

| S-EPMC4525290 | biostudies-literature

Light-driven hydrogen evolution catalyzed by a cobaloxime catalyst incorporated in a MIL-101(Cr) metal-organic framework.

Project description:A cobaloxime H2 evolution catalyst with a hydroxo-functionalized pyridine ligand, Co(dmgH)2(4-HEP)Cl [dmgH = dimethylglyoxime, 4-HEP = 4-(2-hydroxyethyl)pyridine] was immobilized on a chromium terephthalate metal-organic framework (MOF), MIL-101(Cr), to construct a MOF-catalyst hybrid which displays good photocatalytic H2 evolution activity. The longevity of the cobaloxime catalyst is increased by MOF incorporation, but limited by the stability of the cobalt-pyridine bond under turnover conditions.

| S-EPMC6130847 | biostudies-literature

MIL-161 Metal-Organic Framework for Efficient Au(III) Recovery from Secondary Resources: Performance, Mechanism, and DFT Calculations.

Project description:The recovery of precious metals from secondary resources is significant economically and environmentally. However, their separation is still challenging because they often occur in complex metal ion mixtures. The poor selectivity of adsorbents for gold in complicated solutions prevents further application of adsorption technology. In this study, a Zr-based MOF adsorbent, MIL-161, was synthesized using s-tetrazine dicarboxylic acid (H2STz) as an organic ligand. MIL-161 demonstrated a high adsorption capacity of up to 446.49 mg/g and outstanding selectivity for gold(III) in a simulated electronic waste solution as a result of the presence of sulfur- and nitrogen-containing groups. In addition, the MIL-161 adsorbents were characterized using Fourier transform infrared (FT-IR), field emission scanning electron microscopy (FESEM), thermogravimetric analysis (TG), Brunner-Emment-Teller (BET), and X-ray photoelectron spectroscopy (XPS). Additionally, the adsorption kinetics, isotherms, and thermodynamics of the MOF adsorbents were also thoroughly examined. More importantly, the experimental results and DFT calculations indicate that chelation and electrostatic interactions are the main adsorption mechanisms.

| S-EPMC10384270 | biostudies-literature

Removal of 4-chloro-2-methylphenoxyacetic acid from water by MIL-101(Cr) metal-organic framework: kinetics, isotherms and statistical models.

Project description:Effective removal of 4-chloro-2-methylphenoxyacetic acid (MCPA), an emerging agrochemical contaminant in water with carcinogenic and mutagenic health effects has been reported using hydrothermally synthesized MIL-101(Cr) metal-organic framework (MOF). The properties of the MOF were ascertained using powdered X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, thermal gravimetric analysis (TGA), field emission scanning electron microscopy (FESEM) and surface area and porosimetry (SAP). The BET surface area and pore volume of the MOF were 1439 m2 g-1 and 0.77 cm3 g-1, respectively. Artificial neural network (ANN) model was significantly employed for the accurate prediction of the experimental adsorption capacity (qe ) values with minimal error. A rapid removal of the pollutant (99%) was recorded within short time (approx. 25 min), and the reusability of the MOF (20 mg) was achieved up to six cycles with over 90% removal efficiency. The kinetics, isotherm and thermodynamics of the process were described by the pseudo-second-order, Freundlich and endothermic adsorption, respectively. The adsorption process is spontaneous based on the negative Gibbs free energy values. The significant correlation between the experimental findings and simulation results suggests the great potential of MIL-101(Cr) for the remediation of MCPA from water matrices.

| S-EPMC7890509 | biostudies-literature

Effect of solvent nature on propylene glycol oxidation with <i>tert</i>-butyl hydroperoxide over metal-organic framework Cr-MIL-101.

Project description:The effect of solvent nature on conversion, product yields and reaction kinetics of selective propylene glycol oxidation with tert-butyl hydroperoxide over porous chromium terephthalate Cr-MIL-101 used as a heterogeneous catalyst is considered. Differences in hydrogen bonding of propylene glycol molecules in different solvents and adsorption of components of the reaction mixture on the active sites of the catalyst are studied by Fourier-transformed infrared spectroscopy. The characteristics of the solvent are shown to play a key role in the process under consideration. In the case of aprotic solvents, the oxidant utilization efficiency, the propylene glycol conversion and the product yields are significantly higher in comparison with those in protic solvents. The protic solvents can adsorb on the active sites of the catalyst which leads to a decrease of their accessibility for the reagents. The initial rate of propylene glycol oxidation decreases linearly with the increasing of the diameter of molecules of the protic solvents. DFT calculations support the competitive adsorption of the molecules of protic solvents on Cr active sites of MIL-101. In the aprotic solvents, the reactivity and distribution of propylene glycol molecules in the solution are determined by the involvement of hydroxyl groups of the substrate into the intermolecular interactions. The ability of the aprotic solvents to break the hydrogen bond network in the associates of propylene glycol is responsible for the concentration of the substrate molecules in the pores of Cr-MIL-101. The highest selectivities towards hydroxyacetone for Cr-MIL-101 catalyst are obtained in solvents, where the initial rates of propylene glycol oxidation are the lowest ones.

| S-EPMC9070363 | biostudies-literature

Palladium Supported on Porous Organic Polymer as Heterogeneous and Recyclable Catalyst for Cross Coupling Reaction.

Project description:Palladium immobilized on an amide and ether functionalized porous organic polymer (Pd@AEPOP) is reported to be an effective heterogeneous catalyst for the Heck cross-coupling reaction of aryl iodides with styrene for the synthesis of diphenylethene derivatives. Excellent yields can be obtained using a 0.8 mol% Pd catalyst loading under the optimized reaction condition. The heterogeneous Pd@AEPOP catalyst can also be applied on the Suzuki reaction and the reduction of nitroarene.

| S-EPMC9332046 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data