Synthesis of SAPO-34 Nanoplates with High Si/Al Ratio and Improved Acid Site Density.

Two-dimensional SAPO-34 molecular sieves were synthesized by microwave hydrothermal process. The concentrations of structure directing agent (SDA), phosphoric acid, and silicon in the gel solution were varied and their effect on phase, shape, and composition of synthesized particles was studied. The synthesized particles were characterized by various techniques using SEM, XRD, BET, EDX, and NH3-TPD. Various morphologies of particles including isotropic, hyper rectangle, and nanoplates were obtained. It was found that the Si/Al ratio of the SAPO-34 particles was in a direct relationship with the density of acid sites. Moreover, the gel composition and preparation affected the chemistry of the synthesized particles. The slow addition of phosphoric acid improved the homogeneity of synthesis gel and resulted in SAPO-34 nanoplates with high density of acid sites, 3.482 mmol/g. The SAPO-34 nanoplates are expected to serve as a high performance catalyst due to the low mass transfer resistance and the high density of active sites.

Two-Dimensional MFI Zeolite Nanosheets Exfoliated by Surfactant Assisted Solution Process.

Two-dimensional (2D) zeolite nanosheets are important for the synthesis of high flux zeolite membranes due to their lateral size in a preferred orientation. A way to obtain 2D zeolite nanosheets is to exfoliate interlocked structures generated during the hydrothermal synthesis. The mechanical and polymer assisted exfoliation process leads to mechanical damage in nanosheets and short lateral size. In the present study, polyvinylpyrrolidone (PVP) was introduced as an exfoliation agent and dispersant, so that multilamellar interlocked silicalite-1 zeolite nanosheets successfully exfoliated into a large lateral size (individual nanosheets 500~1200 nm). The good exfoliation behavior was due to the strong penetration of PVP into multilamellar nanosheets. Sonication assisted by mild milling helps PVP molecules to penetrate through the lamellar structure, contributing to the expansion of the distance between adjacent layers and thus decreasing the interactions between each layer. In addition, the stability of exfoliated nanosheets was evaluated with a series of organic solvents. The exfoliated nanosheets were well dispersed in n-butanol and stable for 30 days. Therefore, the PVP-assisted solution-based exfoliation process provides high aspect ratio MFI zeolite nanosheets in organic solvents for a long period.

Prevention in Thermal Crack Formation in Chabazite (CHA) Zeolite Membrane by Developing Thin Top Zeolite and Thick Intermediate Layers.

Chabazite (CHA) zeolite membranes with an intermediate layer of various thicknesses were prepared using planetary-milled seeds with an average particle diameter of 300, 250, 200, 140, and 120 nm. The 120 nm seed sample also contained several smaller particles with a diameter of 20 nm. Such small seeds deeply penetrated into the pore channels of the α-alumina support during the vacuum-assisted infiltration process. During the secondary growth, the penetrated seeds formed a thick intermediate layer exiting between the zeolite layer and support. A decrease in seed size increased the penetration depth of seeds and the thickness of the intermediate layer, while the thickness of seed coating and zeolite layers was decreased. CHA zeolite membranes with a thin top zeoliate layer and a thick intermediate layer showed an excellent water/ethanol separation factor (>10,000) for 90 wt.% ethanol at 70 ℃ with a total flux of 1.5 kg m-2 h-1. There was no observation of thermal cracks/defects on the zeolite separation layer. The thick intermediate layer effectively suppressed the formation of thermal cracks during heating, since the tensile stress induced in the zeolite layer was well compensated by the compressive stress on the support. Therefore, it was successfully proven that controlling the microstructure of top surface and intermediate layers is an effective approach to improve the thermal stability of the CHA zeolite membrane.

A stable polymeric chain configuration producing high performance PEBAX-1657 membranes for CO2 separation.

Although PEBAX-1657 is one of the promising polymeric materials for selective CO2 separation, there remain many questions about the optimal polymeric structure and possibility of improving performance without adulterating its basic structure by impregnating inorganic fillers. In order to improve the gas separation performance, low thickness PEBAX membranes were synthesized under steady solvent evaporation conditions by keeping in mind that one of its segments (nylon 6) shows structural variance and molecular orientation with a change in the evaporation rate. Furthermore, phase pure zeolite nanocrystals with cubic (zeolite A) and octahedral (zeolite Y) shapes have been synthesized through liquid phase routes using microwave hydrothermal reactors. The average sizes of zeolite A and Y crystals are around 55 and 40 nm, respectively. The inspection of XRD, DSC and Raman shift of PEBAX membranes demonstrates the formation of a stable polymeric structure with an improved crystalline state which results in high CO2 permeability membranes. The CO2 permeability as well as diffusivity increase with a decrease in membrane thickness and reach a maximum value of 184.7 Barrer and 2.6 × 10-6 cm2 s-1, respectively. The as-fabricated pristine PEBAX membrane shows much better performance in terms of permeance (CO2 184.7 Barrer), diffusivity (CO2 2.6 × 10-6 cm2 s-1) and selectivity (CO2/N2 59.7), which substantiate its promising prospects for CO2 capture. This exceptional performance of the pristine PEBAX membrane arises from the free volume generated during the steady polymerization. This reported approach for PEBAX membrane synthesis provides a direction in the design of membrane fabrication processes for economic CO2 separation.