Fast microwave-assisted preparation of nickel-copper-chromium-layered double hydroxide as an excellent electrocatalyst for water oxidation.

Herein, we describe a simple microwave method for the doping of Cu2+ into NiCr-LDH and the preparation of ternary Ni2.25Cu0.75Cr-LDH as a superior electrocatalyst for water oxidation in a neutral solution. The obtained Ni2.25Cu0.75Cr-LDH was characterized by XRD, DRS, TEM and FE-SEM techniques. The results showed that Ni2.25Cu0.75Cr-LDH was formed with a size of 30 nm. In order to examine the water oxidation activity of Ni2.25Cu0.75Cr-LDH, the as-prepared samples were used as an electrocatalyst-modified carbon paste electrode in neutral solution. The electrochemical results revealed that the optimized Ni2.25Cu0.75Cr-LDH presented extraordinary water oxidation activity with a low onset potential of 1.40 V (vs. RHE) and an overpotential of 170 mV compared to other molar ratios (Ni2.5Cu0. 5Cr-LDH), (Ni2CuCr-LDH), and bimetallic (CuCr-LDH), and even outperformed NiCr-LDH. Also, a small Tafel slope of 31 mV and high durability of 14 h could be obtained for Ni2.25Cu0.75Cr-LDH. The excellent OER could be assigned to the decreased band gap energy and increased charge transfer at Ni2.25Cu0.75Cr-LDH. Therefore, Ni2.25Cu0.75Cr-LDH is a promising water oxidation catalyst owing to its improved charge transfer ability.

Ultrasonication construction of the nano-petal NiCoFe-layered double hydroxide: An excellent water oxidation electrocatalyst.

Unlike other preparation methods of NiCoFe-layered double hydroxides, the present study provides a facile ultrasound method for synthesis of the nano-petal NiCoFe-layered double hydroxide (LDH) prepared under intensification frequency of 40 kHz and ultrasonic power of 305 W. The effect of time reaction on the morphology of NiCoFe-LDH was investigated using the Field Emission-Scanning Electron Microscopy images. The results show that time reaction can affect the morphology and it also showed that the optimal time for synthesis of nano-petal NiCoFe-LDH was 60 min. Then, the effect of nano-petal NiCoFe-LDH on oxygen evaluation reaction activity was studied and compared with NiCoFe-LDH-c nano paricles. Also, in order to study the effect of Co2+ of nano-petal NiCoFe-LDH at water oxidation, the activity of NiFe-LDH synthesized in the same conditions was investigated. The results show that nano-petal NiCoFe-LDH has low onset potential (0.46 V vs. SCE), overpotential (~227 mV) and Tafel slope (234 mV per decade) in comparison with other NiCoFe-LDH nanoparticles (synthesis using co-precipitation method and ultrasonication method within 30 and 120 min), and NiFe-LDH. Based on the obtained results, the nano-petal NiCoFe-LDH can be as a suitable electrocatalyst with good stability for water oxidation reaction in the present 0.1 M KOH media.

Ni-Ti Layered Double Hydroxide@Graphitic Carbon Nitride Nanosheet: A Novel Nanocomposite with High and Ultrafast Sonophotocatalytic Performance for Degradation of Antibiotics.

Pollution of water resources by antibiotics is a growing environmental concern. In this work, nanocomposites of g-C3N4@Ni-Ti layered double hydroxides (g-C3N4@Ni-Ti LDH NCs) with high surface areas were synthesized through an optimized hydrothermal method, in the presence of NH4F. Application of various characterization techniques unraveled that the prepared nanocomposites are composed of porous Ni-Ti LDH nanoparticles and hierarchical g-C3N4 nanosheets. Further, these NCs were employed for photocatalytic and sonophotocatalytic removal of amoxicillin (AMX), as a model antibiotic, from aqueous solutions. In addition, sonocatalysis was performed. It was found out that the g-C3N4@Ni-Ti LDH NCs outperform their pure g-C3N4 and Ni-Ti LDH components in photocatalytic degradation of AMX under visible light irradiation. Also, the following order was determined for efficiency of the three adopted processes: sonocatalysis < photocatalysis < sonophotocatalysis. Furthermore, variation of the sonophotocatalysis conditions specified 500 W light intensity, 9 s on/1 s off ultrasound pulse modem and 1.25 g/L g-C3N4-20@Ni-Ti LDH as the optimal conditions. In this way, optimization of the highly efficient sonophotocatalytic process resulted in 99.5% AMX degradation within 75 min. Moreover, a TOC analyzer was employed to estimate the rate of AMX degradation over the nanocomposites. In addition, formation of hydroxyl radicals (•OH) on the surface of the g-C3N4-20@Ni-Ti LDH particles was approved using the terephthalic acid probe in photoluminescence (PL) spectroscopy. No significant loss was observed in the sonophotocatalytic activity of the nanocomposites even after five consecutive runs. Also, a plausible mechanism was proposed for the sonophotocatalysis reaction. In general, our findings can be considered as a starting point for synthesis of other g-C3N4-based NCs and application of the resultant nanocomposites to environmental remediation.

Ultrasound-assisted synthesis of NiFe- layered double hydroxides as efficient electrode materials in supercapacitors.

Under ultrasound irradiation, NiFe-layered double hydroxide (NiFe-LDH) nanostructures with three molar ratios and three dissimilar reaction times were prepared. The powder X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), and Fourier transform infrared spectroscopy (FT-IR) were employed to characterize the synthesized nanomaterials. Using a sonochemichal route, various morphologies of the NiFe-LDH nanostructures without any impurity and variations in the structure were produced. During the optimization process, it was found that sonication time and reagent concentration in a fixed irradiation frequency can affect the size and the morphology of the produced nanostructures. Under ultrasound irradiation, non-aggregated particles with uniform, spherical morphology were obtained with molar ratios of 4:1 (Ni:Fe) with 45 W at 180 min. The NiFe-LDH samples were observed to be supercapacitor under a 6 M KOH solution. When morphologically-controlled NiFe-LDH samples were used, the pseudo-capacitive behavior of the nanostructures was tuned. After 3 h of ultrasonic irradiation, the optimized sample (NiFe-LDH spherical nanostructures with 4:1 M ratio) had a high value of specific capacitance (168F g-1).

New insights into the interstratification phenomenon in layered double hydroxides (LDHs): a comparison of experimental and computational results for ZnAl-LDH containing bis-tetrazole.

In the present paper, successful preparation of ZnAl layered double hydroxides (LDHs) containing bis-tetrazole anions with both typical and interstratified arrangements is reported. The mechanism of the single-anion interstratified arrangement remains a long-standing and overwhelming challenge in the chemistry of LDHs. To address this issue, the arrangement of layers, the positioning of anions in the interlayer space, and the cationic ratio of layers were studied by the application of a series of laboratory methods including X-ray diffraction (XRD), thermal analyses (TGA, DTG, and DTA), elemental analysis (CHN), and energy dispersive X-ray (EDX) methods, together with computer simulations performed by using Dmol3, Forcite, and Reflex modules. The obtained information demonstrated the dependence of interstratification on the type, size, and charge distribution of the intercalated anions, and the cationic ratio of the LDH layers. At the end, a new comprehensive mechanism is proposed for single-anion interstratification in layered double hydroxides by considering the results of this research study and other related works.

Synthesis and characterization of graphene quantum dots/CoNiAl-layered double-hydroxide nanocomposite: Application as a glucose sensor.

In the present work, a novel nanocomposite based on the graphene quantum dots and CoNiAl-layered double-hydroxide was successfully synthesized by co-precipitation method. To achieve the morphological, structural and compositional information, the resulted nanocomposite was characterized by scanning electron microscopy X-ray diffraction, thermal gravimetric analysis, Fourier transform infrared spectroscopy, and photoluminescence. Then, the nanocomposite was used as a modifier to fabricate a modified carbon paste electrode as a non-enzymatic sensor for glucose determination. Electrochemical behavior and determination of glucose at the nanocomposite modified carbon paste electrode were investigated by cyclic voltammetry and chronoamperometry methods, respectively. The prepared sensor offered good electrocatalytic properties, fast response time, high reproducibility and stability. At the optimum conditions, the constructed sensor exhibits wide linear range; 0.01-14.0 mM with a detection limit of 6 µM (S/N = 3) and high sensitivity of 48.717 µAmM-1. Finally, the sensor was successfully applied to determine the glucose in real samples which demonstrated its applicability.

Synthesis and characterization of Mg-Al-layered double hydroxides intercalated with cubane-1,4-dicarboxylate anions.

In the present work, Mg2Al-layered double hydroxide (LDH) intercalated with cubane-1,4-dicarboxylate anions was prepared from the reaction of solutions of Mg(ii) and Al(iii) nitrate salts with an alkaline solution of cubane-1,4-dicarboxylic acid by using the coprecipitation method. The successful preparation of a nanohybrid of cubane-1,4-dicarboxylate(cubane-dc) anions with LDH was confirmed by powder X-ray diffraction, FTIR spectroscopy and thermal gravimetric analysis (TGA). The increase in the basal spacing of LDHs from 8.67 Å to 13.40 Å shows that cubane-dc anions were successfully incorporated into the interlayer space. Thermogravimetric analyses confirm that the thermal stability of the intercalated cubane-dc anions is greater than that of the pure form before intercalation because of host-guest interactions involving hydrogen bonds. The interlayer structure, hydrogen bonding, and subsequent distension of LDH compounds containing cubane-dc anions were shown by molecular simulation. The RDF (radial distribution function), mean square displacement (MSD), and self-diffusion coefficient were calculated using the trajectory files on the basis of molecular dynamics (MD) simulations, and the results indicated that the cubane-dc anions were more stable when intercalated into the LDH layers. A good agreement was obtained between calculated and measured X-ray diffraction patterns and between experimental and calculated basal spacings.

Syntheses, characterization and study of the use of cobalt (II) Schiff-base complexes as catalysts for the oxidation of styrene by molecular oxygen.

Schiff-Base complexes of bis-5-phenylazosalicylaldehyde ethylenediimine and bis-5-phenylazosalicylaldehyde-O-phenylenediimine ligands with Co(II) (I and II) have been synthesized and characterized by their IR spectra and elemental analyses. These complexes catalyze the oxidation of styrene in the presence of dioxygen and excess pyridine. The effect of the reaction conditions on the oxidation of styrene was studied by varying solvent, nature and amount of the catalyst and substrate. The catalytic behavior of the studied complexes was shown to be dependent on the conditions applied. In all reactions, acetophenone and 1- phenylethanol were the only observed products.