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<p>This work introduces four mutually reinforcing synthesis routes to prepare hydrophobic silicalite-1 zeolite membranes tailored for H₂/CO₂ separation in the presence of moisture. In combination, sequential zirconia intermediate layer, dual-sized seeding, variable-temperature hydrothermal crystallization, and cationic-linker-assisted seeding limit Al leaching from the support, promote the order arrangement of seeds, and drive the formation of continuous, defect-free crystals. Structural and morphological analyses, together with gas permeation tests, verify that the resulting films are dense, highly crystalline, and strongly water-repellent. The best-performing membrane shows a Si/Al ratio of 211 (values commonly reported for Al-containing MFI membranes Si/Al &lt; 100), a water contact angle of 155° (vs. &lt; 120° for conventional layers), and an H₂/CO₂ selectivity of 6.4 while maintaining high permeance. The observed separation behavior closely follows the degree of hydrophobicity, highlighting the critical roles of suppressing Al incorporation and eliminating intercrystalline voids. Overall, the proposed scalable synthesis route yields mechanically robust membranes suitable for post-Water Gas Shift hydrogen upgrading and integration into high-temperature membrane reactors.</p>

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Silicalite-1 hollow fiber zeolite membranes for hydrogen separation from CO₂ under humid conditions

  • 期刊论文

  • 发表日期：

    2026年6月19日

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  • Seyed Mojtaba Mirfendereski,
  • Tayebeh Mazaheri

摘要

This work introduces four mutually reinforcing synthesis routes to prepare hydrophobic silicalite-1 zeolite membranes tailored for H₂/CO₂ separation in the presence of moisture. In combination, sequential zirconia intermediate layer, dual-sized seeding, variable-temperature hydrothermal crystallization, and cationic-linker-assisted seeding limit Al leaching from the support, promote the order arrangement of seeds, and drive the formation of continuous, defect-free crystals. Structural and morphological analyses, together with gas permeation tests, verify that the resulting films are dense, highly crystalline, and strongly water-repellent. The best-performing membrane shows a Si/Al ratio of 211 (values commonly reported for Al-containing MFI membranes Si/Al < 100), a water contact angle of 155° (vs. < 120° for conventional layers), and an H₂/CO₂ selectivity of 6.4 while maintaining high permeance. The observed separation behavior closely follows the degree of hydrophobicity, highlighting the critical roles of suppressing Al incorporation and eliminating intercrystalline voids. Overall, the proposed scalable synthesis route yields mechanically robust membranes suitable for post-Water Gas Shift hydrogen upgrading and integration into high-temperature membrane reactors.