Investigation of Oil-Water Separation on an F-SiO2/TiO2-Based Superhydrophobic/Superoleophilic Surface: Experiment Evaluation and MD Simulation.

Experiment evaluation and mechanism analysis of separation performance are crucial for oily wastewater treatment. In this work, a fluorinated superhydrophobic/superoleophilic (F-SHPB/SOPL) surface was fabricated on a steel mesh substrate by double depositions of SiO2-TiO2 nanoparticles for high-roughness improvement and composite modification of fluorine-alkyl groups for low-energy achievement. Measurements of SEM, XPS, FTIR, laser scanning confocal microscope (LSCM), and excitation-emission matrix (EEM) were carried out for surface property characterization. The oil-water separation performances at the prepared F-SHPB/SOPL surface were investigated from experimental and simulation aspects. Separation tests, flux tests, and anti-contamination tests were performed by experimental methods. The results indicated that the surface showed excellent separation efficiencies (>99.2%) for oil-water mixture and oil-in-water emulsion, high permeate flux (>3000 L·m-2·h-1) for organic oils, and perfect anti-pollution/self-cleaning capacity for liquid and solid contaminations. The interaction energies and interaction distances were measured by ab initio molecular dynamics simulation (AIMD) simulations. With lower interaction energy (Eoil = -456.52∼-1044.22 eV) than that of water molecules (Ewater = -172.73 eV) and shorter distance (Doil = 4.42∼5.13 Å) than that of water molecules (Dwater = 11.49 Å), oil molecules showed higher interaction stability than water molecules on the F-SHPB/SOPL surface. The calculation revealed the essence of the oil-water separation phenomenon. This work not only proposes the fabrication methodology of the SHPB/SOPL material but also elucidates the intermolecular interaction for oil-water separation. The results can provide a fundamental basis for separation operation and removal treatment in industrial and domestic applications.

Insight into Organic Pollutant Adsorption Characteristics on a g-C3N4 Surface by Attenuated Total Reflection Spectroscopy and Molecular Dynamics Simulation.

Herein the adsorption characteristics of zwitterionic dye pollutant Rhodamine B (Rh+B-) on a g-C3N4 surface were investigated by both an attenuated total reflection spectroscopy (ATRS) experiment and a molecular dynamics simulation (MDS). For experimental investigation, g-C3N4 was coated on a silica optical fiber (SOF) surface to fabricate an adsorption film. According to the ATRS response, adsorption thermodynamics and thermodynamics results were in situ obtained and evaluated. The isothermal Langmuir model was used to calculate the adsorption equilibrium constants (Kads) and adsorption energies (ΔGads) for Rh+B- as 27.25 × 104 M-1 and -31.01 kJ mol-1, respectively, which indicated the spontaneous adsorption behavior of Rh+B- at the g-C3N4 surface. Using dynamic Elovich modeling, the rate constants of Rh+B- were found to be k1 = 0.0063 min-1 and k2 = 0.0004 min-1, which indicated two-stage adsorption at the g-C3N4 surface. For theoretical simulation, adsorption configurations and adsorption energies were systematically calculated by a molecular dynamics simulation (MDS) . Rh+B- molecules were inclined to orient in a parallel position at the g-C3N4 surface during low concentration but a perpendicular position at the g-C3N4 surface during high concentration. Combined with experimental and calculation results, this work revealed the microscopic adsorption performance and elucidated the intermolecular interaction between localized interfaces of g-C3N4 and hazardous dye pollutant. We propose an adsorption model to explain the process of surface interaction, which is based on molecular orientation and a force-driven mechanism. Electrostatic attraction and π-π interaction dominated the adsorption interaction with an adsorption energy of ΔGlow(ads) = -38.96 kJ mol-1 for low Rh+B- concentration, and electrostatic attraction dominated the adsorption interaction with an adsorption energy of ΔGhigh(ads) = -25.76 kJ mol-1 for high Rh+B- concentration. This work can provide a fundamental basis for a dye-pollutants removal application by g-C3N4 in both adsorption and photocatalyzation.

Preparation, self-assembly, and mechanistic study of highly monodispersed nanocubes.

In this paper, we describe the synthesis and growth mechanism of highly monodispersed platinum nanocubes. The platinum nanocubes are synthesized by the decomposition of a platinum precursor in a hydrogen atmosphere. The morphology and size distribution of the platinum particles formed has been studied with HRTEM. By controlling the concentration of the platinum precursor, we demonstrate that at low concentration, it is possible to grow polydispersed nanocubes with {1,0,0} facets. Increasing the concentration of the precursor changes the growth mechanism, resulting in the formation of highly monodispersed platinum nanocubes. Highly monodispersed platinum nanocubes are formed in a two-step growth mechanism with initial growth of the {1,1,1} facets followed by secondary growth filling the {1,0,0} facets. The particle monodispersity facilitates the formation of long-range arrays of nanocubes.