Metal–Site Dispersed Zinc–Chromium Oxide Derived from Chromate–Intercalated Layered Hydroxide for Highly Selective Propane Dehydrogenation
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PROVIDER: S-EPMC11243157 | biostudies-literature | 2024 Jun
REPOSITORIES: biostudies-literature
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Project description:Mesoporous alumina with narrow pore size distribution centered in the range of 4.4-5.0 nm and with a specific surface area as high as 270 m²·g-1 was prepared via the nanocasting approach using a CMK-3 carbon replica as a hard template. Based on this support, a series of catalysts containing 1, 5, 10, 20 and 30 wt % of chromium was prepared by incipient wetness impregnation, characterized, and studied in the dehydrogenation of propane to propene (PDH). Cr species in three oxidation states-Cr(III), Cr(V) and Cr(VI)-were found on the oxidized surface of the catalysts. The concentration of these species varied with the total Cr loading. Temperature-programmed reduction (H₂-TPR) and UV-Vis diffuse reflectance spectroscopy (UV-Vis-DRS) studies revealed that Cr(VI) species dominated at the lowest Cr content. An increase in the Cr loading resulted in an appearance of an increasing amount of Cr(III) oxide. UV-Vis-DRS measurements performed in situ during the PDH process showed that at the beginning of the catalytic test Cr(VI) species were reduced to Cr(III) redox species. A crucial role of the redox species in the PDH process over the catalysts with the low Cr content was confirmed. The stability test for the catalyst containing 20 wt % of Cr showed that this sample exhibited the reproducible catalytic performance after the first four regeneration-dehydrogenation cycles. Moreover, this catalyst had higher resistance on deactivation during the PDH process as compared to the reference catalyst with the same Cr loading, but was supported on commercially available alumina.
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Project description:Silver oxide nanoparticles with controlled particle size were successfully obtained utilizing citrate-intercalated layered double hydroxide (LDH) as a substrate and Ag+ as a precursor. The lattice of LDH was partially dissolved during the reaction by Ag+. The released hydroxyl and citrate acted as a reactant in crystal growth and a size controlling capping agent, respectively. X-ray diffraction, X-ray photoelectron spectroscopy, and microscopic measurements clearly showed the development of nano-sized silver oxide particles on the LDH surface. The particle size, homogeneity and purity of silver oxide were influenced by the stoichiometric ratio of Ag/Al. At the lowest silver ratio, the particle size was the smallest, while the chemical purity was the highest. X-ray photoelectron spectroscopy and UV-vis spectroscopy results suggested that the high Ag/Al ratio tended to produce silver oxide with a complex silver environment. The small particle size and homogeneous distribution of silver oxide showed advantages in antibacterial efficacy compared with bulk silver oxide. LDH with an appropriate ratio could be utilized as a substrate to grow silver oxide nanoparticles with controlled size with effective antibacterial performance.
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Project description:We found in our previous study that layered double hydroxides (LDHs) which undergo aqueous miscible organic solvent treatment (AMOST) can tune the hydrophobicity surface of LDHs to be hydrophobic, and then the solvent mixing method can be used to prepare polymer/LDH nanocomposites. However, flame retardant property is not very high if LDHs are only used. In this present work, ammonium polyphosphate (APP) intercalated LDHs and zinc borate (ZB) was incorporated into a polypropylene (PP) matrix using the solvent mixing method. The structures, morphologies, and performance of the composites were characterized carefully. The peak heat release rate (PHRR) reduction of PP containing 10 and 20 wt % APP-LDH reached 27% and 55%, respectively, which increased up to 63% compared with PP/CO₃-LDH. After incorporating 2 wt % ZB in the PP/APP-LDH system, the flame retardant property was further improved. Polypropylene composites with 20 wt % APP-LDH and 2 wt % ZB showed a 58% PHRR reduction. In addition, thermogravimetric analyzer (TGA) results indicated that the addition of APP-LDH and ZB improved the temperature at 50% weight loss (T50%) and the char formation of the materials significantly.
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Project description:A layered hydroxide salt (LHS) was used as an inorganic matrix to obtain multifunctional food compounds. The aim is to obtain higher thermal stability for vitamin anions and a slow release of aroma. Thus, vitamin B3 (nicotinate), vitamin B5 (phantothenate) and vitamin L (2-aminobenzoate) anions were intercalated by co-precipitation method. The results show an increase in thermal stability of intercalated vitamin anion since decomposition of pure vitamin B3 starts at 120 °C and after intercalation, the HSL-B3 decomposition starts at 313 °C. The intercalation products were than reacted with vanillin (3-methoxy-4-hydroxybenzaldehyde). A kinetic study showed that the release of vanillin from its nanohybrid was found to occur in a controlled manner, evidencing that the synthesized compounds can be used in formulations for the sustained release of aromas. Results showed that the intercalated anions and adsolubilized vanillin were not only less volatile since it causes the aroma to remain in the LHS for a longer period of time resulting in slow release but also have higher thermal stability when they are confined between layers. In summary, the multifunctional food supplements obtained seems to have nutraceutical, olfactory and better thermal resistance properties being suitable for potential applications in the food industry.
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Project description:In this study, organo-inorganic nanohybrids LHGd-MTSPP with enzyme-like activity were prepared by in situ intercalation of anionic 5,10,15,20-tetrakis-(4-sulfonatophenyl)porphyrin and its complexes with Zn(II) and Pd(II) (MTSPP, M = 2H, Zn(II) and Pd(II)) into gadolinium layered hydroxide (LHGd). The combination of powder XRD, CHNS analysis, FT-IR, EDX, and TG confirmed the layered structure of the reaction products. The basal interplanar distances in LHGd-MTSPP samples were 22.3–22.6 Å, corresponding to the size of an intercalated tetrapyrrole molecule. According to SEM data, LHGd-MTSPP hybrids consisted of individual lamellar nanoparticles 20–50 nm in thickness. The enzyme-like activity of individual constituents, LHGd-Cl and sulfoporphyrins TSPP, ZnTSPP and PdTSPP, and hybrid LHGd-MTSPP materials, was studied by chemiluminescence analysis using the ABAP/luminol system in phosphate buffer solution. All the individual porphyrins exhibited dose-dependent antioxidant properties with respect to alkylperoxyl radicals at pH 7.4. The intercalation of free base TSPP porphyrin into the LHGd preserved the radical scavenging properties of the product. Conversely, in LHGd-MTSPP samples containing Zn(II) and Pd(II) complexes, the antioxidant properties of the porphyrins changed to dose-dependent prooxidant activity. Thus, an efficient approach to the design and synthesis of advanced LHGd-MTSPP materials with switchable enzyme-like activity was developed.
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Project description:In recent years, there has been an increasing interest in stimuli-responsive host-guest materials due to the high potential for their application in switchable devices. Light is the most convenient stimulus for operating these materials; a light-responsive guest affects the host structure and the functional characteristics of the entire material. UV-transparent layered rare earth hydroxides intercalated with UV-switchable anions are promising candidates as stimuli-responsive host-guest materials. The interlayer distance in the layered rare earth hydroxides depends on the size of the intercalated anions, which could be changed in situ, e.g., via anion isomerisation. Nevertheless, for layered rare earth hydroxides, the possibility of such changes has not been reported yet. A good candidate anion that is capable of intercalating into the interlayer space is the cinnamate anion, which undergoes UV-assisted irreversible trans-cis isomerisation. In this work, both trans- and cis-cinnamate anions were intercalated in layered yttrium hydroxide (LYH). Upon UV-irradiation, the interlayer distance of trans-cinnamate-intercalated layered yttrium hydroxide suspended in isopropanol changed from 21.9 to 20.6 Å. For the first time, the results obtained demonstrate the possibility of using layered rare earth hydroxides as stimuli-responsive materials.
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Project description:The aim of this study was to realize the intercalation of the pyrethroid pesticides beta-cypermethrin (BCT) and lambda-cyhalothrin (LCT) into ZnAl-layered double hydroxides (LDH) and NiZn-layered hydroxide salt (LHS). BCT (LCT)/SBECD-LDH and BCT (LCT)/SBECD-LHS hybrids were obtained with the aid of sulfobutyl ether β-cyclodextrin (SBECD) through one step method. The hybrids were characterized by powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and thermogravimetry and differential thermal analysis (TGA/DTA). The hybrids based on LHS had larger basal spacing than those on LDH. The LDH-hybrids prepared in N-methylpyrrolidone (NMP) had larger basal spacing than those in ethanol. These results were discussed in terms of the matrix structure and solvent properties. The supramolecular structure of the hybrid was reasonably proposed. Furthermore, the release properties of BCT (LCT) from the hybrids were investigated and discussed in two media. The release rate in pH = 5.0 was slower than that in pH = 6.8. The accumulated release amount of pesticide in pH = 5.0 was lower than that in pH = 6.8. LHS-hybrids synthesized in ethanol exhibit a sustainable release property. These depend on the inclusion complexes' arrangement and release medium. The release kinetic processes could be described by pseudo-second order and parabolic diffusion models. The release behavior can be controlled by adjusting the synthesis conditions and the releasing media. This provides the guidance for the application of SBECD and LDH (LHS) in pesticide formulation.
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Project description:Herein, magnesium/aluminum-layered double hydroxide (MgAl-LDH) and bentonite (BT) nanocomposites (LDH-BT) were prepared by co-precipitation (CP), exfoliation-reassembly (ER), and simple solid-phase hybridization (SP). The prepared LDH-BT nanocomposites were preliminarily characterized by using powder X-ray diffractometry, scanning electron microscopy, and zeta-potentiometry. The chromate adsorption efficacies of the pristine materials (LDH and bentonite) and the as-prepared nanocomposites were investigated. Among the composites, the LDH-BT_SP was found to exhibit the highest chromate removal efficiency of 65.7%. The effect of varying the LDH amount in the LDH-BT composite was further investigated, and a positive relationship between the LDH ratio and chromate removal efficiency was identified. The chromate adsorption by the LDH-BT_SP was performed under various concentrations (isotherm) and contact times (kinetic). The results of the isotherm experiments were well fitted with the Langmuir and Freundlich isotherm model and demonstrate multilayer chromate adsorption by the heterogeneous LDH-BT_SP, with a homogenous distribution of LDH nanoparticles. The mobility of the as-prepared LDH-BT_SP was investigated on a silica sand-filled column to demonstrate that the mobility of the bentonite is dramatically decreased after hybridization with LDH. Furthermore, when the LDH-BT_SP was injected into a box container filled with silica sand to simulate subsurface soil conditions, the chromate removal efficacy was around 43% in 170 min. Thus, it was confirmed that the LDH-BT prepared by solid-phase hybridization is a practical clay-based nanocomposite for in situ soil and groundwater remediation.
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Project description:2D inorganic materials and their exfoliated counterparts are both of fundamental interest and relevant for applications including catalysis, electronics and sensing. Here, a new bottom-up synthesis route is used to prepare functionalised nanoplatelets, in apolar organic solvents, via the hydrolysis of organometallic reagents; the products can be prepared in high yield, at room temperature. In particular, a series of layered zinc hydroxides, coordinated by aliphatic carboxylate ligands, were produced by the hydrolysis of diethyl zinc and zinc carboxylate mixtures, optimally at a molar ratio of [COOR]/[Zn] = 0.6. Layered zinc hydroxides coordinated by oleate ligands form high concentration solutions of isolated monolayers (3 nm thick x ∼ 26 nm) in apolar organic solvents (up to 23 mg mL-1 in toluene), as confirmed by both atomic force and transmission electron microscopies of deposited species. The high solubility of the product allows the synthetic pathway to be monitored directly in situ through 1H NMR spectroscopy. The high solubility also provides a route to solution deposition of active functional materials, as illustrated by the formation of nanoporous films of optically transparent porous zinc oxide (1 μm thickness) after annealing at 500 °C. This new organometallic route to 2D materials obviates common complications of top-down exfoliation syntheses, including sonochemical-degradation and low yields of aggregated polydispersed layers, and may potentially be extended to a wide range of systems.
| S-EPMC5896490 | biostudies-literature
Project description:Composite hydrogels were prepared that consisted of quasi-colloidal layered double hydroxide (LDH) nanoparticles and agarose via the electrophoretic method, starting from three different agarose concentrations of 0.5, 1, and 2 wt/v%. The composite hydrogel was identified to have a uniform distribution of LDH nanoparticles in agarose matrix. Microscopic studies revealed that the composite hydrogel had a homogeneous quasi-colloidal state of LDHs, while the simple mixture of LDH powder and agarose hydrogels did not. It was determined that agarose concentration of the starting hydrogel did not significantly influence the amount of LDH that developed in the composite. The chromate scavenging efficiency of the composite hydrogel and corresponding agarose or mixture hydrogel was evaluated with respect to time, and chromate concentration. In general, the composite hydrogels exhibited much higher chromate removal efficacy compared with agarose or mixture hydrogels. Through estimating chromate adsorption by LDH moiety in the composite or mixture hydrogel, it was suggested that the agarose component facilitated the stability and dispersibility of the quasi-colloidal state of LDH nanoparticles in the composite resulting in high adsorption efficacy. From Freundlich isotherm adsorption fitting, composites were determined to possess beneficial cooperative adsorption behavior with a high adsorption coefficient.
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