Single gas permeance performance of the high silica SSZ-13 zeolite membrane (Si/Al = 79) was greatly improved by acid post-treatment in this work. Effects of post-treatment conditions, such as post-treatment temperature (25, 60, 80, and 100 °C) and time (0–2 h), acid concentration (0–0.6 H+ mol/L), and acid type (HCl, HNO3, H2SO4, and H3PO4), on the single gas permeance performance of the membrane were investigated in this study. Morphology and structure of the acid post-treated membrane is identical with the fresh high silica SSZ-13 zeolites by advance characterization results, only the amorphous on the zeolites surface is removed and filled into the intercrystalline by medium acid post-treatment, which could improve the gas permeance performance of the membranes greatly. When the post-treatment temperature, time, acid type, and H+ concentration are 25 °C, 0.5 h, H2SO4, and 0.4 mol/L, the CO2/CH4, CO2/N2, H2/CH4, and H2/SF6 ideal selectivity of the post-treated high silica SSZ-13 zeolite membrane are increased to 68, 10, 29, and 126 at 0.2 MPa and 25 °C, respectively.
Continuous and high silica SSZ-13 zeolite membranes were prepared on porous mullite supports from high SiO2/Al2O3 ratio or aluminum-free precursor synthesis gel. Single gas permeance (CO2 and CH4) of the high silica SSZ-13 zeolite membrane was decreased with the SiO2/Al2O3 ratio in the precursor synthesis gel, while the ideal CO2/CH4 selectivity of the membrane was gradually increased. Moreover, effects of synthesis conditions (such as H2O/SiO2 and RNOH/SiO2 ratios of precursor synthesis gel, crystallization time) on the single gas permeance performance of high silica SSZ-13 zeolite membranes were studied in detail. Medium H2O/SiO2 and RNOH/SiO2 ratios in the initial synthesis gel were crucial to prepare the good CO2 perm-selective SSZ-13 zeolite membrane. When the molar composition of precursor synthesis gel, crystallization temperature and time were 1.0 SiO2: 0.1 Na2O: 0.1 TMAdaOH: 80 H2O, 160 °C and 48 h, CO2 permeance and ideal CO2/CH4 selectivity of the SSZ-13 zeolite membrane were 0.98 × 10−7 mol/(m2·s·Pa) and 47 at 25 °C and 0.4 MPa. In addition, the SiO2/Al2O3 ratio of the corresponding SSZ-13 zeolite was 410 by X-ray fluorescence spectroscopy.
In recent years, the utilisation of ionic liquids supported on porous polymer membranes has been demonstrated to enhance gas separation performance by improving both permeability and selectivity for several industrially-relevant gas mixtures. However, the use of such supported ionic liquid membranes (SILMs) is normally not feasible at elevated process temperatures due to the resulting decrease in ionic liquid viscosity, which can lead to increased loss of ionic liquid from the membrane support during operation. In addition, many of the polymer membranes typically used in SILMs exhibit relatively poor mechanical and thermal stabilities at high temperatures. To overcome these problems associated with SILMs, thermally-stable composite ionic liquid and polymer membranes (CILPMs) have been fabricated in this study, thus exploiting the beneficial properties of ionic liquids for gas separation at elevated temperatures. Poly (pyromellitimide-co-4,4-oxydianiline) (PMDA-ODA PI) in combination with the ionic liquid, [C4mi [NTf2] were used to fabricate the CILPMs. A measurement rig was designed and built to determine permeabilities and selectivities of the CILPMs for H2, N2, CO, CO2 and CH4 over a range of pressures and temperatures. The fabricated CILPMs were shown to maintain excellent mechanical and thermal stability over a wide range of processing conditions. Temperature was shown to greatly affect both permeability and selectivity of the membranes, whilst pressure had less influence. The incorporation of [C4mi [NTf2] into the membranes was found to significantly increase CO2 permeation and, therefore, it is anticipated that these CILPMs hold significant potential for CO2 separation applications.
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