Optimization and Synthesis of a La-TMA MOF with Some Improvements in Its Properties
Ontology highlight
ABSTRACT:
SUBMITTER:
PROVIDER: S-EPMC9835621 | biostudies-literature | 2022 Dec
REPOSITORIES: biostudies-literature
Similar Datasets
Project description:Membrane technology plays a vital, applicable, and essential role in human
| S-EPMC10308571 | biostudies-literature
Project description:Metal-organic frameworks (MOFs) were supported on polymer membrane substrates for the fabrication of composite polymer membranes based on unmodified and modified polymer of intrinsic microporosity (PIM-1). Layers of two different MOFs, zeolitic imidazolate framework-8 (ZIF-8) and Copper benzene tricarboxylate ((HKUST-1), were grown onto neat PIM-1, amide surface-modified PIM-1 and hexamethylenediamine (HMDA) -modified PIM-1. The surface-grown crystalline MOFs were characterized by a combination of several techniques, including powder X-ray diffraction, infrared spectroscopy and scanning electron microscopy to investigate the film morphology on the neat and modified PIM-1 membranes. The pure gas permeabilities of He, H₂, O₂, N₂, CH₄, CO₂ were studied to understand the effect of the surface modification on the basic transport properties and evaluate the potential use of these membranes for industrially relevant gas separations. The pure gas transport was discussed in terms of permeability and selectivity, highlighting the effect of the MOF growth on the diffusion coefficients of the gas in the new composite polymer membranes. The results confirm that the growth of MOFs on polymer membranes can enhance the selectivity of the appropriately functionalized PIM-1, without a dramatic decrease of the permeability.
| S-EPMC5371968 | biostudies-literature
Project description:The metal or metal clusters and organic ligands are relevant to the selectivity and performance of phosphate removal in MOFs, and the electron structure, chemical characteristics, and preparation method also affect efficiency and commercial promotion. However, few reports focus on the above, especially for 2D MOF nanomaterials. In this work, two 2D Ln-TDA (Ln = La, Ce) nanosheets assembled via microwave- and ultrasonic-assisted methods are employed as adsorbents for phosphate (H2PO4-, HPO42-) removal for the first time. Their microstructure and performance were characterized using XRD, TEM, SEM, AFM, FTIR, zeta potential, and DFT calculations. The prepared 2D Ln-TDA (Ln = La, Ce) nanosheets exposed more adsorption sites and effectively reduced the restrictions of mass transfer. Based on this, the Langmuir model was employed to estimate the maximum adsorption capacities of the two kinds of nanosheets, which reached 253.5 mg g-1 and 259.5 mg g-1, which are 553 times and 3054 times larger than those for bulk Ln-TDA (Ln = La, Ce), respectively. Additionally, the kinetic data showed that the adsorption equilibrium time is fast, approximately 15 min by the pseudo-second-order model. In addition, the prepared products not only have a wide application range (pH = 3-9) but also offer eco-safety in terms of residuals (no Ln leak out). Based on the XPS spectra, FTIR spectra and DFT calculations, the main adsorption mechanisms included ligand exchange and electrostatic interactions. This new insight provides a novel strategy to prepare 2D MOF adsorbents, achieving a more eco-friendly method (microwave- and ultrasonic-assisted synthesis) for preparing 2D Ln-based MOF nanosheets by coordinative unsaturation to boost phosphate adsorption.
| S-EPMC9743790 | biostudies-literature
Project description:Addressing serious waterborne arsenic issues, for the first time, lanthanum-doped MOF-808 (La@MOF-808) has been developed to remove total arsenic (Total As) and arsenite [As(III)] from water. This study involves the solvothermal synthesis of La@MOF-808, its characterization via FTIR, XRD, TGA, and SEM, in which distinct physicochemical attributes were identified, and the adsorption capacity of arsenic ions. The saturated adsorption capacity of La@MOF-808 for Total As and As(III) reached 282.9 mg g-1 and 283.5 mg g-1, as compared to 229.7 mg g-1 and 239.1 mg g-1 for pristine MOF-808, respectively. XRD and ATR-FTIR analyses underscored the central roles of electrostatic interactions and hydroxyl groups in the pollutant adsorption process. The impact of temperature, concentration, pH, and exposure duration times on adsorption performance was thoroughly investigated. The Langmuir model showed the maximum adsorption capacities (qmax) of La@MOF-808 was 307.7 mg g-1 for Total As and 325.7 mg g-1 for As(III), surpassing those of MOF-808 adsorbent, which suggests that monolayer adsorption occurred. Optimal adsorption was observed in a pH range of 2.0-7.0, and thermodynamic studies classified the process as spontaneous and endothermic. The adsorbent retains high capacity across repeated cycles, outperforming many standard adsorbents. Lanthanum doping markedly enhances MOF-808's arsenic removal, underscoring its potential for water treatment.
| S-EPMC10665691 | biostudies-literature
Project description:Iron-containing metal-organic frameworks are promising Fenton catalysts. However, the absence of additional modifiers has proven difficult due to the low reaction rates and the inability to manipulate the catalysts. We hypothesize that the production of iron oxide NPs in the presence of a metal-organic framework will increase the rate of the Fenton reaction and lead to the production of particles that can be magnetically manipulated without changing the structure of the components. A comprehensive approach lead to a metal organic framework using the example of MIL-88b (Materials of Institute Lavoisier) modified with iron oxides NPs: formulation of iron oxide in the presence of MIL-88b and vice versa. The synthesis of MIL-88b consists of preparing a complexation compound with the respective structure and addition of terephthalic acid. The synthesis of MIL-88b facilitates to control the topology of the resulting material. Both methods for composite formulation lead to the preservation of the structure of iron oxide, however, a more technologically complex approach to obtaining MIL-88b in the presence of Fe3O4 suddenly turned out to be the more efficient for the release of iron ions.
| S-EPMC10958221 | biostudies-literature
Project description:Metal-organic frameworks (MOFs) promise to engender technology-enabling properties for numerous applications. However, one significant challenge in MOF development is their overwhelmingly large design space, which is intractable to fully explore even computationally. To find diverse optimal MOF designs without exploring the full design space, we develop Vendi Bayesian optimization (VBO), a new algorithm that combines traditional Bayesian optimization with the Vendi score, a recently introduced interpretable diversity measure. Both Bayesian optimization and the Vendi score require a kernel similarity function, we therefore also introduce a novel similarity function in the space of MOFs that accounts for both chemical and structural features. This new similarity metric enables VBO to find optimal MOFs with properties that may depend on both chemistry and structure. We statistically assessed VBO by its ability to optimize three NH3-adsorption dependent performance metrics that depend, to different degrees, on MOF chemistry and structure. With ten simulated campaigns done for each metric, VBO consistently outperformed random search to find high-performing designs within a 1000-MOF subset for (i) NH3 storage, (ii) NH3 removal from membrane plasma reactors, and (iii) NH3 capture from air. Then, with one campaign dedicated to finding optimal MOFs for NH3 storage in a "hybrid" ∼10 000-MOF database, we identify twelve extant and eight hypothesized MOF designs with potentially record-breaking working capacity ΔN NH3 between 300 K and 400 K at 1 bar. Specifically, the best MOF designs are predicted to (i) achieve ΔN NH3 values between 23.6 and 29.3 mmol g-1, potentially surpassing those that MOFs previously experimentally tested for NH3 adsorption would have at the proposed operation conditions, (ii) be thermally stable at the operation conditions and (iii) require only ca. 10% of the energy content in NH3 to release the stored molecule from the MOF. Finally, the analysis of the generated simulation data during the search indicates that a pore size of around 10 Å, a heat of adsorption around 33 kJ mol-1, and the presence of Ca could be part of MOF design rules that could help optimize NH3 working capacity at the proposed operation conditions.
| S-EPMC11499977 | biostudies-literature
Project description:This work reports on the ultrasonic synthesis of layered double hydroxides (LDH), also known as hydrotalcite-type materials. We have studied the influence of ultrasonic irradiation parameters (power, time, temperature) on the physicochemical properties of Ni2Mg4Al1.8La0.2 hydrotalcite-type precursors and related mixed oxides (MO). The low-frequency acoustic cavitation (22 kHz) was applied during the precipitation and aging steps of co-precipitation synthesis and the results were compared to the classical preparation route. The materials were characterized by ATR-FTIR, XRD, N2 adsorption-desorption, SEM-EDX, S/TEM-HAADF, and XPS. Using the combination of acoustic cavitation-assisted precipitation and aging steps, XRD experiments show a higher purity hydrotalcite phase and a better incorporation of lanthanum ions into the LDH structure. As expected, morphological characterization shows a reduction in average crystallite size and an increase in surface area and pore volume, combined with a drastic reduction in synthesis time (45 min at room temperature versus 19 h at 60 °C in conventional synthesis). The insertion of a larger quantity of La is observed by S/TEM-EDSX mapping which also shows a better distribution of lanthanum atoms within the LDH and mixed oxide structures.
| S-EPMC10884977 | biostudies-literature
Project description:While the overwhelming number of papers on multi-principal-element alloys (MPEAs) focus on the mechanical and microstructural properties, there has been growing interest in these alloys as solid-state hydrogen stores. We report here the synthesis optimization, the physicochemical and the hydrogen sorption properties of Ti0.325V0.275Zr0.125Nb0.275. This alloy was prepared by two methods, high temperature arc melting and ball milling under Ar, and crystallizes into a single-phase bcc structure. This MPEA shows a single transition from the initial bcc phase to a final bct dihydride and a maximum uptake of 1.7 H/M (2.5 wt%). Interestingly, the bct dihydride phase can be directly obtained by reactive ball milling under hydrogen pressure. The hydrogen desorption properties of the hydrides obtained by hydrogenation of the alloy prepared by arc melting or ball milling and by reactive ball milling have been compared. The best hydrogen sorption properties are shown by the material prepared by reactive ball milling. Despite a fading of the capacity for the first cycles, the reversible capacity of the latter material stabilizes around 2 wt%. To complement the experimental approach, a theoretical investigation combining a random distribution technique and first principle calculation was done to estimate the stability of the hydride.
| S-EPMC6695880 | biostudies-literature
Project description:Monodisperse spherical silica particles, with solid cores and mesoporous shells (SCMS), were synthesized at various temperatures using a one-pot method utilizing a cationic surfactant template. The temperature of the synthesis was found to significantly affect the diameters of both the cores (ca. 170-800 nm) and shells (ca. 11-80 nm) of the particles, which can be tailored for specific applications that require a high specific surface area of the nanocarriers (mesoporous shells) and simultaneously their mechanical robustness for, e.g., facile isolation from suspensions (dense cores). The applied method enabled the formation of the relatively thick mesoporous shells at conditions below room temperature. Radially ordered pores with narrow distributions of their sizes in 3-4 nm range were found in the shells. The adsorption ability of the SCMS particles was studied using rhodamine 6G as a model dye. Decolorization of the dye solution in the presence of the SCMS particles was correlated with their structure and specific surface area and reached its maximum for the particles synthesized at 15 °C. The presented strategy may be applied for the fine-tuning of the structure of SCMS particles and the enhancement of their adsorption capabilities.
| S-EPMC5923560 | biostudies-literature
Project description:Mechanochemical synthesis has recently emerged as a scalable "green" approach for the preparation of MOFs, but current understanding of the underlying reaction mechanisms is limited. In this work, an investigation of the reaction pathway of the mechanochemical synthesis of MOF-74 from ZnO and 2,5-dihydroxyterephthalic acid (H4HDTA), using DMF as a liquid additive, is presented. The complex reaction pathway involves the formation of four short-lived intermediate phases, prior to the crystallization of MOF-74. The crystal structures of three of these intermediates have been determined using a combination of single-crystal and powder X-ray diffraction methods and are described here. The initial stages of the reaction are very fast, with a DMF solvate of H4HDTA forming after only 2 min of milling. This is followed by crystallization, after only 4 min of milling, of a triclinic one-dimensional coordination polymer, Zn(H2DHTA)(DMF)2(H2O)2, which converts into a monoclinic polymorph on additional milling. Highly crystalline MOF-74 appears after prolonged milling, for at least 70 min.
| S-EPMC8273859 | biostudies-literature