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<p>This study investigates the effect of amine types on the structure of organosilica materials for CO<sub>2</sub> separation. The materials were synthesized using primary (3-amino propyl triethoxy silane (APTES)), secondary (bis-[3-(trimethoxysilyl) propyl] amine (BTPA)), and tertiary (tris (3-trimethoxysilyl propyl) amine (TTPA)) precursors, differing in linking units and alkoxy group numbers. These materials show high stability and improved CO<sub>2</sub> separation. Preliminary optimization was conducted on BTPA to determine the best type of acid catalyst, water-to-silane mole ratio, and catalyst-to-silane mole ratio. Material characterization was performed using FTIR, XRD, TGA, N<sub>2,</sub> and CO<sub>2</sub> adsorption-desorption isotherms. The results revealed that a weak acid catalyst (acetic acid-HAc) produced a less stable Si-O-Si framework, while HNO<sub>3</sub> formed more ordered frameworks. A water-mole ratio of 50 was needed for complete hydrolysis of one alkoxy group; thus, ratios of 150, 300, and 450 were used for APTES (3-alkoxy), BTPA (6-alkoxy), and TTPA (9-alkoxy), respectively. Higher acid ratios accelerated the formation of well-ordered Si-O-Si frameworks. CO<sub>2</sub> capture evaluations showed that the secondary amine of BTPA exhibited the highest CO<sub>2</sub> adsorption due to enhanced interaction and carbamate formation, followed by APTES &gt; TTPA. APTES showed better CO<sub>2</sub>/N<sub>2</sub> separation at low pressures due to lower steric hindrance and smaller membrane pore size, which improves the adsorption ability and separation. The membrane performance is in agreement with material characterization, which shows CO<sub>2</sub> permeance of 2.1 <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(\times\)</EquationSource> <EquationSource Format="MATHML"><math> <mo>×</mo> </math></EquationSource> </InlineEquation> 10<sup>-8 </sup>mol m<sup>−2</sup> s<sup>−1</sup> Pa<sup>−1</sup> and the highest CO<sub>2</sub>/N<sub>2</sub> separation of 17 for APTES. This study provides insights into optimizing amine-functionalized organosilica for efficient CO<sub>2</sub>/N<sub>2</sub> separation. The optimized membranes show promising potential for efficient industrial CO<sub>2</sub>/N<sub>2</sub> separation performance, offering competitive performance relative to commercially available membrane technology.</p><p></p>

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Investigation of CO2/N2 separation capabilities for various amine-functionalized organosilica membranes: synthesis and sorption study evaluation

  • 期刊论文

  • 发表日期：

    2025年9月9日

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  • Ufafa Anggarini,
  • Deviana Rahayu,
  • Fauzul Azizah Oktaviola,
  • Ndaru Candra Sukmana,
  • Wei Wei Yan,
  • Hiroki Nagasawa,
  • Toshinori Tsuru,
  • Masakoto Kanezashi

摘要

This study investigates the effect of amine types on the structure of organosilica materials for CO2 separation. The materials were synthesized using primary (3-amino propyl triethoxy silane (APTES)), secondary (bis-[3-(trimethoxysilyl) propyl] amine (BTPA)), and tertiary (tris (3-trimethoxysilyl propyl) amine (TTPA)) precursors, differing in linking units and alkoxy group numbers. These materials show high stability and improved CO2 separation. Preliminary optimization was conducted on BTPA to determine the best type of acid catalyst, water-to-silane mole ratio, and catalyst-to-silane mole ratio. Material characterization was performed using FTIR, XRD, TGA, N2, and CO2 adsorption-desorption isotherms. The results revealed that a weak acid catalyst (acetic acid-HAc) produced a less stable Si-O-Si framework, while HNO3 formed more ordered frameworks. A water-mole ratio of 50 was needed for complete hydrolysis of one alkoxy group; thus, ratios of 150, 300, and 450 were used for APTES (3-alkoxy), BTPA (6-alkoxy), and TTPA (9-alkoxy), respectively. Higher acid ratios accelerated the formation of well-ordered Si-O-Si frameworks. CO2 capture evaluations showed that the secondary amine of BTPA exhibited the highest CO2 adsorption due to enhanced interaction and carbamate formation, followed by APTES > TTPA. APTES showed better CO2/N2 separation at low pressures due to lower steric hindrance and smaller membrane pore size, which improves the adsorption ability and separation. The membrane performance is in agreement with material characterization, which shows CO2 permeance of 2.1 \(\times\) × 10-8 mol m−2 s−1 Pa−1 and the highest CO2/N2 separation of 17 for APTES. This study provides insights into optimizing amine-functionalized organosilica for efficient CO2/N2 separation. The optimized membranes show promising potential for efficient industrial CO2/N2 separation performance, offering competitive performance relative to commercially available membrane technology.