Pore size tuning of bis(triethoxysilyl)propane (BTESP)-derived membrane for gas separation: Effects of the acid molar ratio in the sol and of the calcination temperature

Inoue, Ryota; Kanezashi, Masakoto; Nagasawa, Hiroki; Yamamoto, Kazuki; Gunji, Takahiro; Tsuru, Toshinori

doi:10.1016/j.seppur.2020.116742

Cited by 9 publications

(6 citation statements)

References 63 publications

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“…Since these membranes were prepared via different preparation processes and materials, the performances were scattered as shown in SI‐5 (Supporting Information). The reproducibility of each membrane type can be found elsewhere 23‐29 . H 2 permeance ranged from 2.1 × 10 −8 (TiPCS‐2) to 3.2 × 10 −6 mol/(m 2 s Pa) (BTESA‐1).…”

Section: Resultsmentioning

confidence: 98%

“…1,2‐bis(triethoxysilyl)ethane (BTESE), 1,2‐bis(triethoxysilyl)propane (BTESP) and 1,2‐bis(triethoxysilyl)acetylene (BTESA) were used as precursors for BTESE‐, BTESP‐, and BTESA‐derived sols. The preparation process for BTESE‐, 31 BTESP‐, 25 and BTESA‐ 26 derived sols have been reported in detail elsewhere. Briefly, each precursor was mixed with ethanol, water and hydrochloric acid, and then stirred at 50°C.…”

Section: Methodsmentioning

confidence: 99%

“…Details for the preparation of BTESE‐, 31 BTESP‐, 25 BTESA‐, 26 AHPCS‐, 28 and TiPCS‐ 29 derived membranes are reported elsewhere. In brief, tuber membranes were composed of three layers that included a support, an intermediate layer, and a separation layer.…”

Section: Methodsmentioning

confidence: 99%

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Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation

et al. 2021

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Pervaporation (PV) is a membrane technology that holds great promise for industrial applications. To better understand the PV mechanism, PV dehydrations of various types of organic solvents (methanol, ethanol, iso‐propanol, tert‐butanol, and acetone) were performed on five types of organosilica and two types of silicon carbide‐based membranes, all with different pore sizes. Water permeance was dependent on the types of organic aqueous solutions, which suggested that organic solvents penetrated the pores and hindered the permeation of water. In addition, water permeance of various types of membranes in PV was well correlated with hydrogen permeance in single‐gas permeation. Furthermore, a clear correlation was obtained between the permeance ratio in PV and that in single‐gas permeation, which was confirmed via the modified‐gas translation model. These correlations make it possible to use single‐gas permeation properties to predict PV performance.

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Section: Resultsmentioning

confidence: 98%

Section: Methodsmentioning

confidence: 99%

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Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation

et al. 2021

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“…The incorporation of fluorine into hydrophobic pendant–type organosilica further improved the hydrophobic/hydrophilic properties. Several studies have reported similar results of increased hydrophobicity with the addition of fluoride ions into silica matrix by showing the very low amount of H 2 O adsorbed by comparison with undoped samples [ 26 , 36 , 37 ].…”

Section: Resultsmentioning

confidence: 64%

The Effect of C/Si Ratio and Fluorine Doping on the Gas Permeation Properties of Pendant-Type and Bridged-Type Organosilica Membranes

et al. 2022

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A series of pendant–type alkoxysilane structures with various carbon numbers (C1–C8) were used to fabricate sol–gel derived organosilica membranes to evaluate the effects of the C/Si ratio and fluorine doping. Initially, this investigation was focused on the effect that carbon-linking (pendant–type) units exert on a microporous structure and how this affects the gas-permeation properties of pendant–type organosilica membranes. Gas permeation results were compared with those of bridged–type organosilica membranes (C1–C8). Network pore size evaluation was conducted based on the selectivity of H2/N2 and the activation energy (Ep) of H2 permeation. Consequently, Ep (H2) was increased as the C/Si ratio increased from C1 to C8, which could have been due to the aggregation of pendant side chains that occupied the available micropore channel space and resulted in the reduced pore size. By comparison, these permeation results indicate that pendant–type organosilica membranes showed a somewhat loose network structure in comparison with bridged–type organosilica membranes by following the lower values of activation energies (Ep). Subsequently, we also evaluated the effect that fluorine doping (NH4F) exerts on pendant−type [methytriethoxysilane (MTES), propyltrimethoxysilane (PTMS)] and bridged-type [1,2–bis(triethoxysilyl)methane (BTESM) bis(triethoxysilyl)propane (BTESP)] organosilica structures with similar carbon numbers (C1 and C3). The gas-permeation properties of F–doped pendant network structures revealed values for pore size, H2/N2 selectivity, and Ep (H2) that were comparable to those of pristine organosilica membranes. This could be ascribed to the pendant side chains, which might have hindered the effectiveness of fluorine in pendant–type organosilica structures. The F–doped bridged–type organosilica (BTESM and BTESP) membranes, on the other hand, exhibited a looser network formation as the fluorine concentration increased.

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“…Porous silica membranes exhibit high thermal, chemical, and mechanical stabilities compared with polymer-based membranes that tend to show a decline in performance under harsh conditions (e.g., high-temperature and/or high-pressure conditions) due to the possible degradation, swelling, and plasticization of polymers. − Tetraetoxysilane-derived SiO 2 membranes fabricated via sol–gel methods can easily form a thin separation layer so that these membranes show high levels of permeance and selectivity, which is particularly suitable for the separation of small gases such as H 2 (H 2 /N 2 and CO 2 /H 2 ). ,− Moreover, bridged-type organosilica membranes with controlled pore sizes by changing the linking units have been applied to separation systems that range from liquid to gas separation. ,− For CO 2 separation systems such as CO 2 /N 2 and CO 2 /CH 4 , however, it is difficult to tune the network pore size based on the molecular sieving mechanism since these gases have similar kinetic diameters (CO 2 : 0.33 nm, N 2 : 0.364 nm, and CH 4 : 0.38 nm). Thus, controlling the interactions with CO 2 is as important as controlling the pore size to achieve a high level of CO 2 separation performance.…”

Section: Introductionmentioning

confidence: 99%

Pore Structure Controllability and CO₂ Permeation Properties of Silica-Derived Membranes with a Dual-Network Structure

Nakahiro

Nagasawa

et al. 2021

Ind. Eng. Chem. Res.

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We proposed a novel method for designing CO2 permselective organosilica/polymer membranes with a dual-network structure composed of silica (first) and alkylamine-based (second) networks to control molecular sieving and CO2 adsorption properties in the membrane. Organosilica/polymer membranes were fabricated using 1,2-bis(triethoxysilyl)ethane (BTESE) or 1,2-bis(triethoxyailyl)acetylene (BTESA) as the first network, with polyethylenimine (PEI) as the second network via the sol–gel process. CO2 adsorption measurements of BTESE/PEI films were conducted via in situ Fourier transform infrared to evaluate the effects that different types of acid catalysts exert on CO2 adsorption properties. The results showed that only BTESE/PEI films prepared with a catalyst of acetic acid (HAc) display impressive chemical reactions between CO2 and amine groups, whereas the use of HCl may deactivate the amine groups. We found that the gas permeation properties of organosilica/PEI membranes were greatly dependent on the Si-precursor. Almost no selectivity could be confirmed for BTESA/PEI membranes, although pure BTESA membranes did show molecular sieving properties. However, BTESE/PEI membranes showed improved separation performance compared with that of pure BTESE membranes due to a reduction in the free volume (BTESE: H2/CH4 selectivity < 100, BTESE/PEI: H2/CH4 > 100). Moreover, the pore size of BTESE/PEI membranes could be controlled via the BTESE/PEI ratio. In conclusion, we successfully designed a dual-network structure with a controlled pore size via changes made to the Si-precursor and/or to the Si-precursor/PEI mixing ratio.

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Pore size tuning of bis(triethoxysilyl)propane (BTESP)-derived membrane for gas separation: Effects of the acid molar ratio in the sol and of the calcination temperature

Cited by 9 publications

References 63 publications

Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation

Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation

The Effect of C/Si Ratio and Fluorine Doping on the Gas Permeation Properties of Pendant-Type and Bridged-Type Organosilica Membranes

Pore Structure Controllability and CO₂ Permeation Properties of Silica-Derived Membranes with a Dual-Network Structure

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Pore size tuning of bis(triethoxysilyl)propane (BTESP)-derived membrane for gas separation: Effects of the acid molar ratio in the sol and of the calcination temperature

Cited by 9 publications

References 63 publications

Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation

Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation

The Effect of C/Si Ratio and Fluorine Doping on the Gas Permeation Properties of Pendant-Type and Bridged-Type Organosilica Membranes

Pore Structure Controllability and CO2 Permeation Properties of Silica-Derived Membranes with a Dual-Network Structure

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Product

Resources

About

Pore Structure Controllability and CO₂ Permeation Properties of Silica-Derived Membranes with a Dual-Network Structure