RESUMEN
Electrochemical approaches for generating hydrogen from water splitting can be more promising if the challenges in the anodic oxygen evolution reaction (OER) can be harnessed. The interface heterostructure materials offer strong electronic coupling and appropriate charge transport at the interface regions, promoting accessible active sites to prompt kinetics and optimize the adsorption-desorption of active species. Herein, we have designed an efficient multi-interface-engineered Ni3Fe1 LDH/Ni3S2/TW heterostructure on in situ generated titanate web layers from the titanium foam. The synergistic effects of the multi-interface heterostructure caused the exposure of rich interfacial electronic coupling, fast reaction kinetics, and enhanced accessible site activity and site populations. The as-prepared electrocatalyst demonstrates outstanding OER activity, demanding a low overpotential of 220 mV at a high current density of 100 mA cm-2. Similarly, the designed Ni3Fe1 LDH/Ni3S2/TW electrocatalyst exhibits a low Tafel slope of 43.2 mV dec-1 and excellent stability for 100 h of operation, suggesting rapid kinetics and good structural stability. Also, the electrocatalyst shows a low overpotential of 260 mV at 100 mA cm-2 for HER activity. Moreover, the integrated electrocatalyst exhibits an incredible OER activity in simulated seawater with an overpotential of 370 mV at 100 mA cm-2 and stability for 100 h of operation, indicating good OER selectivity. This work might benefit further fabricating effective and stable self-sustained electrocatalysts for water splitting in large-scale applications.
RESUMEN
Currently, hydrogen peroxide (H2O2) manufacturing involves an energy-intensive anthraquinone technique that demands expensive solvent extraction and a multistep process with substantial energy consumption. In this work, we synthesized Pd-N4-CO, Pd-S4-NCO, and Pd-N2O2-C single-atom catalysts via an in situ synthesis approach involving heteroatom-rich ligands and activated carbon under mild reaction conditions. It reveals that palladium atoms interact strongly with heteroatom-rich ligands, which provide well-defined and uniform active sites for oxygen (O2) electrochemically reduced to hydrogen peroxide. Interestingly, the Pd-N4-CO electrocatalyst shows excellent performance for the electrocatalytic reduction of O2 to H2O2 via a two-electron transfer process in a base electrolyte, exhibiting a negligible amount of onset overpotential and >95% selectivity within a wide range of applied potentials. The electrocatalysts based on the activity and selectivity toward 2e- ORR follow the order Pd-N4-CO > Pd-N2O2-C > Pd-S4-NCO in agreement with the pull-push mechanism, which is the Pd center strongly coordinated with high electronegativity donor atoms (N and O atoms) and weakly coordinated with the intermediate *OOH to excellent selectivity and sustainable production of H2O2. According to density functional theory, Pd-N4 is the active site for selectivity toward H2O2 generation. This work provides an emerging technique for designing high-performance H2O2 electrosynthesis catalysts and the rational integration of several active sites for green and sustainable chemical synthesis via electrochemical processes.
RESUMEN
In the present research, the kaolin adsorbents (beneficiated, raw powder, and calcined) were prepared from Ethiopian natural kaolin through mechanical, wet, and thermal processes. The geochemical and surface properties of kaolin adsorbent were characterized using FTIR, SEM/EDS, XRD, and XRF. In the batch experiment, basic operation parameters (initial dye concentrations, pH, temperature, contact time, and adsorbent dosage) were examined. Percentage removal efficiency basic yellow 28 (BY28) dye were recorded as 94.79%, 92.08%, and 87.08% onto beneficiated, raw, and calcined kaolin absorbents, respectively at an initial dye concentration of 20 mg/L, solution pH of 9, the temperature of 30 °C °C , and contact time of 60 min and adsorbent dosage of 1g/100L. The molar ratio of SiO2/Al2O3 was recorded as 2.911 Percent mass composition of Ethiopian kaolin which is higher than the expected pure kaolinite standard which allows us to classify the kaolin clay as a siliceous one. The calculated values of Δ G 0 for beneficiated adsorbent are -1.243, 1.576, and 4.396 kJ/mol at 303.15, 323.15, and 343.15 K, respectively for 20 mg/L of dye concentration and solution pH of 9, suggests that the thermodynamic behavior at lowest temperature is more feasible and spontaneous as compared with the higher temperature one. A similar fashion was calculated for raw and calcined adsorbents. The negative values of ΔHo and ΔS° suggest that the adsorption phenomenon is exothermic and the adsorbate molecules are organized on the solid phase in a more disordered fashion than the liquid phase. The pseudo-first-order and pseudo-second-order models have been used to describe the kinetics in the adsorption processes. The Pseudo-second-order model has been fitted for the BY 28 dye adsorption in the studied concentration range. The adsorption of BY 28 dye for raw and calcined adsorbents follows the Langmuir isotherm and the Freundlich isotherm fitted for the beneficiated adsorbent. The amount of BY28 dye taken up by beneficiated, raw, and calcined kaolin adsorbents was found as 1.896, 1.842, and 1.742 mg/g, respectively at a contact time of 1.0 h, the adsorbent dosage of 1.0 g, initial dye concentration = 20 mg/L and solution pH = 9 at 30 °C. The results found that these raw and prepared local kaolin adsorbents have a capacity as low-cost alternatives for the removal of dyes in industrial wastewater.
RESUMEN
This article presents batch experimental data describing the main batch adsorption operation parameters. Also the adsorption models (adsorption isotherm, adsorption kinetics and thermodynamic studies) of basic yellow dye on to the raw and treated kaolin adsorbents. Besides, instrumental analyses were recorded to characterize kaolin adsorbent. Such as, thermogravimetric analyzer, Fourier transformation infrared and scanning electroscope with energy dispersion spectroscopy were used. UV-Visible spectrometer was used throughout the experimental study for the determination of absorbance. The effect of adsorption temperature (30 °C, 50 °C 70 °C), PH (3, 7, 9), initial dye concentration (20 mg/l, 40 mg/l, 60 mg/l), contact time (20 min, 40 min, 60 min, 80 min, 100 min) and adsorbent dosage (0.1, 0.5, 1, 1.5, 2 g/100ml) have been well determined. For adsorbent characteristics, we provide dataset regarding (i) thermogravimetery with differential scanning calorimetery, (ii) Fourier transform infrared spectral data before and after basic yellow dye adsorption process, (iii) scanning electroscope with energy dispersion spectroscopy image at ×500 resolution, (iv) X-ray diffraction and, (v) batch adsorption experimental parameters records. Regarding scanning electroscope with energy dispersion spectroscopy image, we provide data of three surface morphology image and three elemental distribution spectra for raw and treated kaolin adsorbent.
