Abstract
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.
Highlights
As a high-quality, clean fuel and important chemical raw materials, natural gas has attracted a lot of attention recently
A high silica SSZ-13 zeolite membrane was synthesized on the porous mullite tubes by secondary hydrothermal synthesis
The water adsorption property of zeolite membrane greatly depended on the SiO2 /Al2 O3 ratio of of membrane layer, and the hydrophobicity of the zeolite membrane was increased with the membrane layer, and the hydrophobicity of the zeolite membrane was increased with the SiO2 /Al2 O3
Summary
As a high-quality, clean fuel and important chemical raw materials, natural gas has attracted a lot of attention recently. CO2 content of natural gas was high in general, which could have a great influence on the combustion heat of natural gas. The high CO2 content natural gas would corrode the steel pipeline and increase the transportation equipment costs. Amine adsorption and cryogenic distillation are the main technologies for CO2 capture and separation, which are the energy-intensive and cost-intensive processes [3]. Membrane separation was expected to be a novel and energy efficient technology for CO2 capture and separation, which was no need for sorbent regeneration or desorption [4]. Baker et al reported that polymeric membranes could separate CO2 from natural gas [5]. The high CO2 pressure could plasticize polymeric membranes and decrease separation performance of polymeric membranes [6].
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