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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.
Keita Nakahiro; Liang Yu; Hiroki Nagasawa; Toshinori Tsuru; Masakoto Kanezashi. Pore Structure Controllability and CO2 Permeation Properties of Silica-Derived Membranes with a Dual-Network Structure. Industrial & Engineering Chemistry Research 2021, 60, 8527 -8537.
AMA StyleKeita Nakahiro, Liang Yu, Hiroki Nagasawa, Toshinori Tsuru, Masakoto Kanezashi. Pore Structure Controllability and CO2 Permeation Properties of Silica-Derived Membranes with a Dual-Network Structure. Industrial & Engineering Chemistry Research. 2021; 60 (23):8527-8537.
Chicago/Turabian StyleKeita Nakahiro; Liang Yu; Hiroki Nagasawa; Toshinori Tsuru; Masakoto Kanezashi. 2021. "Pore Structure Controllability and CO2 Permeation Properties of Silica-Derived Membranes with a Dual-Network Structure." Industrial & Engineering Chemistry Research 60, no. 23: 8527-8537.
The nickel-doped bis [3-(trimethoxysilyl) propyl] amine (BTPA) derived membrane has a microporous coordinated network that has high potential to be an ideal separation barrier for methanol-toluene azeotropic mixtures via the pervaporation process. Ni-BTPA membranes were modified by employing a nickel dopant over amine groups in mole ratios (mol/mol) that ranged from 0.125 to 0.50. The incorporation of different amounts of nickel dopant into flexible amine-rich organosilica precursors of BTPA increased the rigidity and resulted in a porous structure with a large specific surface area (increased from 2.36 up to 282 m2 g–1) and a high pore volume (from 0.024 up to 0.184 cm3 g–1). Methanol-toluene separation performance by the nickel-doped BTPA (Ni-BTPA) membranes was increased with increases in the nickel concentration. Ni-BTPA 0.50 showed separation performance that was superior to other types of membranes, along with a high-level of flux at 2.8 kg m–2 h–1 and a separation factor higher than 900 in a 10 wt % methanol feed solution at 50 °C. These results suggest that the balance between the microporosity induced by amine-nickel coordination and an excessive amount of nickel-ion facilitates high levels of flux and separation of methanol.
Ufafa Anggarini; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. Microporous Nickel-Coordinated Aminosilica Membranes for Improved Pervaporation Performance of Methanol/Toluene Separation. ACS Applied Materials & Interfaces 2021, 13, 23247 -23259.
AMA StyleUfafa Anggarini, Liang Yu, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. Microporous Nickel-Coordinated Aminosilica Membranes for Improved Pervaporation Performance of Methanol/Toluene Separation. ACS Applied Materials & Interfaces. 2021; 13 (19):23247-23259.
Chicago/Turabian StyleUfafa Anggarini; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2021. "Microporous Nickel-Coordinated Aminosilica Membranes for Improved Pervaporation Performance of Methanol/Toluene Separation." ACS Applied Materials & Interfaces 13, no. 19: 23247-23259.
Hybrid microporous aminosilica membranes have been successfully synthesized via doping with Ag-, Cu- and Ni-into dense bis[3-(trimethoxysilyl)propyl] amine (BTPA) membranes, which creates micropores via the crosslinking between donor pairs of electrons in the amine moiety and electron acceptors in the empty “d” orbital of a transition metal.
Ufafa Anggarini; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. Metal-induced microporous aminosilica creates a highly permeable gas-separation membrane. Materials Chemistry Frontiers 2021, 5, 3029 -3042.
AMA StyleUfafa Anggarini, Liang Yu, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. Metal-induced microporous aminosilica creates a highly permeable gas-separation membrane. Materials Chemistry Frontiers. 2021; 5 (7):3029-3042.
Chicago/Turabian StyleUfafa Anggarini; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2021. "Metal-induced microporous aminosilica creates a highly permeable gas-separation membrane." Materials Chemistry Frontiers 5, no. 7: 3029-3042.
The evolution of the physicochemical properties of allylhydridopolycarbosilane (AHPCS) was systematically investigated via DLS, TG, FTIR, XRD, and EDS. AHPCS-derived membranes were prepared by coating AHPCS sols onto porous substrates, which was then followed by pyrolysis at 300–800 °C. The pre-crosslinking by thermal curing significantly increased the colloidal sol size of AHPCS in toluene solutions, which effectively reduced penetration into substrates and enhanced the gas permeation. Furthermore, the pore structure of AHPCS-derived membranes could be precisely tailored by the pyrolysis temperatures, and the results indicated that the structure of membranes could be roughly classified into one of three types: a dense polymer structure, a loose transitional structure, and a denser ceramic structure (here, the term ‘dense/denser’ refers to the small/smaller pore structure, while the ‘loose’ refers to the large pore structure). AHPCS-derived membranes prepared at 300–800 °C under a N2 flow displayed superior H2 permeance of (0.2–5) × 10−6 mol/(m2 s Pa) at 200 °C with good H2/N2 selectivity of 12–56. Ceramic SiC membranes prepared at 700 °C showed an attractive H2 permeance of (2–4) × 10−6 mol (m2 s Pa)−1 at 200 °C with H2/N2 selectivity of 16–22, H2/SF6 selectivity higher than 10,000, and N2/SF6 selectivity higher than 800. Moreover, the structure of the ceramic SiC membranes was highly stable with good oxidation resistance at 500 °C under air. AHPCS membranes prepared at 300–800 °C had different pore structures that exhibited a high level of quality and a variety of permeation properties that could provide many options for membrane materials over a wide range of applications.
Qing Wang; Makoto Yokoji; Hiroki Nagasawa; Liang Yu; Masakoto Kanezashi; Toshinori Tsuru. Microstructure evolution and enhanced permeation of SiC membranes derived from allylhydridopolycarbosilane. Journal of Membrane Science 2020, 612, 118392 .
AMA StyleQing Wang, Makoto Yokoji, Hiroki Nagasawa, Liang Yu, Masakoto Kanezashi, Toshinori Tsuru. Microstructure evolution and enhanced permeation of SiC membranes derived from allylhydridopolycarbosilane. Journal of Membrane Science. 2020; 612 ():118392.
Chicago/Turabian StyleQing Wang; Makoto Yokoji; Hiroki Nagasawa; Liang Yu; Masakoto Kanezashi; Toshinori Tsuru. 2020. "Microstructure evolution and enhanced permeation of SiC membranes derived from allylhydridopolycarbosilane." Journal of Membrane Science 612, no. : 118392.
Membrane-based separation technologies are considered an effective process for the capture of CO2 due to advantages such as high levels of energy efficiency with inexpensive levels of investment. It remains challenging, however, to develop a membrane with high levels of both permeance and selectivity with the ability to capture CO2 in a highly efficient manner. Herein, we report amino-decorated organosilica membranes that are based on a facile and effective co-polymerization strategy that uses bis(triethoxysilyl)acetylene (BTESA) and (3-aminopropyl) triethoxysilane (APTES) precursors. This co-polymerization strategy simultaneously endows the resultant membranes with a controlled pore size and enhanced CO2-philic properties that have significantly improved CO2 separation performance. These composite membranes display CO2 permeance that ranges from 2550–3230 GPU and a range for CO2/N2 selectivity of 31–42 in the separation of CO2/N2 mixtures, which outperforms most state-of-the-art membranes and exceeds the target for post-combustion CO2 capture operations. A satisfying performance was achieved with a CO2 permeance of 8 ✕ 10−7 mol m−2 s−1 Pa−1 (2390 GPU) and CO2/CH4 selectivity of 70. The present study highlights an elegant decoration strategy for the production of membranes with ultrahigh CO2 capture capacities, which can also be extended to other organosilica precursors for target-oriented separations by varying the bridged or side-chain groups.
Meng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Joji Ohshita; Toshinori Tsuru. Amino-decorated organosilica membranes for highly permeable CO2 capture. Journal of Membrane Science 2020, 611, 118328 .
AMA StyleMeng Guo, Masakoto Kanezashi, Hiroki Nagasawa, Liang Yu, Joji Ohshita, Toshinori Tsuru. Amino-decorated organosilica membranes for highly permeable CO2 capture. Journal of Membrane Science. 2020; 611 ():118328.
Chicago/Turabian StyleMeng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Joji Ohshita; Toshinori Tsuru. 2020. "Amino-decorated organosilica membranes for highly permeable CO2 capture." Journal of Membrane Science 611, no. : 118328.
Membrane-based separation of organic/organic mixtures is of great importance in the chemical and petrochemical industries, but remains very challenging owing to the harsh working conditions. Herein, ultrathin and chemically stable Bis(triethoxysilyl)acetylene (BTESA)-derived organosilica membranes were reproducibly prepared, and for the first time they were utilized in the pervaporation separation of methanol/organic azeotropes. The as-prepared BTESA membranes exhibited exceptional pervaporation performance in a 10 wt%/90 wt% methanol/dimethyl carbonate (DMC) mixture, and showed a high separation factor of approximately 120 with a permeation flux of 2–4 kg m-2 h-1 at 50 °C. This impressive performance was primarily the result of the preferential sorption of methanol and the efficient size sieving of DMC. In addition, the effects of feed concentration and temperature on methanol/DMC pervaporation performance were thoroughly investigated. Importantly, a generalized solution-diffusion model successfully described the pervaporation performance of BTESA membranes, and the usefulness of this model was further confirmed via the pervaporation of methanol/methyl acetate and methanol/methyl tert-butyl ether (MTBE) mixtures. This work demonstrates the great potential of organosilica membranes for high-performance organic/organic pervaporation.
Guanying Dong; Hiroki Nagasawa; Liang Yu; Qing Wang; Kazuki Yamamoto; Joji Ohshita; Masakoto Kanezashi; Toshinori Tsuru. Pervaporation removal of methanol from methanol/organic azeotropes using organosilica membranes: Experimental and modeling. Journal of Membrane Science 2020, 610, 118284 .
AMA StyleGuanying Dong, Hiroki Nagasawa, Liang Yu, Qing Wang, Kazuki Yamamoto, Joji Ohshita, Masakoto Kanezashi, Toshinori Tsuru. Pervaporation removal of methanol from methanol/organic azeotropes using organosilica membranes: Experimental and modeling. Journal of Membrane Science. 2020; 610 ():118284.
Chicago/Turabian StyleGuanying Dong; Hiroki Nagasawa; Liang Yu; Qing Wang; Kazuki Yamamoto; Joji Ohshita; Masakoto Kanezashi; Toshinori Tsuru. 2020. "Pervaporation removal of methanol from methanol/organic azeotropes using organosilica membranes: Experimental and modeling." Journal of Membrane Science 610, no. : 118284.
In this study, the physicochemical properties and microstructural variations of polycarbosilane (PCS) were systematically investigated at curing temperatures of 150–350 °C and pyrolysis temperatures of 350–850 °C. Oxidative cross-linking remarkably enhanced the thermal stability of the PCS structure. Elemental composition and microstructure of the final ceramic material could be precisely tailored via the air curing process. Cross-linking by air curing that is either excessive or insufficient could cause the micropores of the resulting ceramic material to collapse or disappear. The most promising PCS-derived membranes, which were cured at 250 °C and then pyrolyzed at 750 °C, had high thermal stability and oxidation resistance at 500 °C in addition to excellent permeation properties: H2 permeance of 1–2 × 10−6 mol/(m2 s Pa) at 500 °C with H2/N2 selectivity of 31 and H2/C3H8 selectivity of 1,740; and, CO2 permeance of 1.8 × 10−6 mol/(m2 s Pa) at 27 °C with CO2/CH4 selectivity of 40. Moreover, permeance and selectivity in an equimolar H2/C3H8 mixture at 500 °C were approximately the same as those in single gases, suggesting the separation mechanism could be ascribed to molecular sieving. This is the first study to propose the concept of tailoring the microstructure of SiC-based membranes by controlling the curing process.
Qing Wang; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. Tuning the microstructure of polycarbosilane-derived SiC(O) separation membranes via thermal-oxidative cross-linking. Separation and Purification Technology 2020, 248, 117067 .
AMA StyleQing Wang, Liang Yu, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. Tuning the microstructure of polycarbosilane-derived SiC(O) separation membranes via thermal-oxidative cross-linking. Separation and Purification Technology. 2020; 248 ():117067.
Chicago/Turabian StyleQing Wang; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2020. "Tuning the microstructure of polycarbosilane-derived SiC(O) separation membranes via thermal-oxidative cross-linking." Separation and Purification Technology 248, no. : 117067.
Polytitanocarbosilane (TiPCS)‐derived ceramic membranes were fabricated using a pre‐ceramic polymer. Special attention was focused on a process of thermal‐oxidative curing that was used to induce cross‐linking and the effect of this process on the ceramic yield, thermal stability, oxidation resistance, and microstructure of TiPCS. The cross‐linked TiPCS powders showed a ceramic yield and thermal stability that were higher than that from the non‐cross‐linked version. In addition, the cross‐linked TiPCS with uniform micropores showed higher levels of N2 and CO2 adsorption capacity, BET surface area, and micropore volume than the non‐cross‐linked versions, and the cross‐linking process enhanced the stability of the pore structure at high temperature. The cross‐linked TiPCS membranes showed high H2 permeance (1.49×10‐6 mol/(m2 s Pa)) with sub‐nanopores (H2/SF6 selectivity: 12,000, H2/N2: 10), and in addition higher oxidation resistance than their non‐cross‐linked counterparts. Furthermore, the influence of the concentration of the TiPCS precursor coating solution was optimized and the hydrothermal stability of the membranes at high temperatures were also evaluated. The optimized membrane demonstrated great performance for the pervaporation removal of methanol in binary azeotropic systems of either MeOH/butyl acetate or MeOH/toluene, and it also showed high hydrothermal stability with excellent dehumidification performance under high temperatures.
Qing Wang; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. High‐performance molecular‐separation ceramic membranes derived from oxidative cross‐linked polytitanocarbosilane. Journal of the American Ceramic Society 2020, 103, 4473 -4488.
AMA StyleQing Wang, Liang Yu, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. High‐performance molecular‐separation ceramic membranes derived from oxidative cross‐linked polytitanocarbosilane. Journal of the American Ceramic Society. 2020; 103 (8):4473-4488.
Chicago/Turabian StyleQing Wang; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2020. "High‐performance molecular‐separation ceramic membranes derived from oxidative cross‐linked polytitanocarbosilane." Journal of the American Ceramic Society 103, no. 8: 4473-4488.
Membrane-based separation techniques are responsible for great advances in the separation of propylene/propane mixtures. In this study, bis(triethoxysilyl)acetylene (BTESA) was selected as the precursor in the fabrication of organosilica membranes for use in propylene/propane separation. We proposed an effective strategy to finely engineer the pore subnano-environment of BTESA membranes for highly selective propylene/propane separation via controlling the calcination temperatures. Measurement of the surface energy, the 29Si-NMR spectra, and the gas sorption isotherms clearly indicated that low-temperature calcined BTESA materials with a greater number of silanol groups showed an enhanced affinity to propylene molecules. BTESA membranes calcined at 150 °C featured a promisingly high C3H6/C3H8 selectivity of 52 and a C3H6 permeance of 1.7 ✕ 10−8 mol m−2 s−1 Pa−1 at 50 °C. These values were approximate to those reported for ZIF-8 membranes and higher than the standards for commercialization. The high level of C3H6/C3H8 separation performance was believed to be accounted by the synergetic effects of both controlled pore size and enhanced affinity to propylene molecules. Moreover, compared with traditional organosilica membranes that were calcined at ~350 °C, low-temperature calcination (150 °C) for BTESA membranes efficiently reduced the energy consumption and fabrication cost.
Meng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Kazuki Yamamoto; Takahiro Gunji; Joji Ohshita; Toshinori Tsuru. Pore subnano-environment engineering of organosilica membranes for highly selective propylene/propane separation. Journal of Membrane Science 2020, 603, 117999 .
AMA StyleMeng Guo, Masakoto Kanezashi, Hiroki Nagasawa, Liang Yu, Kazuki Yamamoto, Takahiro Gunji, Joji Ohshita, Toshinori Tsuru. Pore subnano-environment engineering of organosilica membranes for highly selective propylene/propane separation. Journal of Membrane Science. 2020; 603 ():117999.
Chicago/Turabian StyleMeng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Kazuki Yamamoto; Takahiro Gunji; Joji Ohshita; Toshinori Tsuru. 2020. "Pore subnano-environment engineering of organosilica membranes for highly selective propylene/propane separation." Journal of Membrane Science 603, no. : 117999.
Liang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. Phase inversion/sintering-induced porous ceramic microsheet membranes for high-quality separation of oily wastewater. Journal of Membrane Science 2020, 595, 1 .
AMA StyleLiang Yu, Masakoto Kanezashi, Hiroki Nagasawa, Toshinori Tsuru. Phase inversion/sintering-induced porous ceramic microsheet membranes for high-quality separation of oily wastewater. Journal of Membrane Science. 2020; 595 ():1.
Chicago/Turabian StyleLiang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. 2020. "Phase inversion/sintering-induced porous ceramic microsheet membranes for high-quality separation of oily wastewater." Journal of Membrane Science 595, no. : 1.
We developed a procedure that saves significant amounts of energy during the separation of organic liquids via organic solvent reverse osmosis (OSRO). The proof-of-concept was confirmed using theoretical calculation to demonstrate energy-consumption at less than 1/100th and 1/10th that of conventional distillation and pervaporation (PV), respectively. Bis(triethoxysilyl)acetylene (BTESA)-derived organosilica membranes consisting of a SiO2–ZrO2 intermediate layer and an α-Al2O3 support were evaluated by challenging a series of azeotropic mixtures of methanol/toluene, methanol/methyl acetate, methanol/dimethyl carbonate (DMC), and methanol/methyl tert-butyl ether (MTBE). BTESA membranes showed excellent size- and/or shape-sieving properties and remarkable levels of organic-tolerance with an ultrahigh methanol flux that outperforms state-of-the-art polymeric membranes. In particular, the robust ceramic support and rigid organosilica networks endowed the resultant membranes with the ability to withstand transmembrane pressures as high as 18 MPa.
Guanying Dong; Hiroki Nagasawa; Liang Yu; Meng Guo; Masakoto Kanezashi; Tomohisa Yoshioka; Toshinori Tsuru. Energy-efficient separation of organic liquids using organosilica membranes via a reverse osmosis route. Journal of Membrane Science 2019, 597, 117758 .
AMA StyleGuanying Dong, Hiroki Nagasawa, Liang Yu, Meng Guo, Masakoto Kanezashi, Tomohisa Yoshioka, Toshinori Tsuru. Energy-efficient separation of organic liquids using organosilica membranes via a reverse osmosis route. Journal of Membrane Science. 2019; 597 ():117758.
Chicago/Turabian StyleGuanying Dong; Hiroki Nagasawa; Liang Yu; Meng Guo; Masakoto Kanezashi; Tomohisa Yoshioka; Toshinori Tsuru. 2019. "Energy-efficient separation of organic liquids using organosilica membranes via a reverse osmosis route." Journal of Membrane Science 597, no. : 117758.
The separation of azeotropic mixtures such as methyl acetate and methanol via a membrane is an interesting and challenging issue, since the membrane must be able to withstand these harsh solvents and provide good flux and selectivity. SiC-based membranes have attracted a great deal of interest due to their high mechanical strength, structural stability, and corrosion resistance at elevated temperatures. Herein, we describe the first use of polytitanocarbosilane (TiPCS), which is known as a precursor of continuous Si–Ti–C–O fibers (Tyranno), in the preparation of Ti-incorporated SiC-based membranes for the pervaporation (PV) removal of water or methanol, and describe the evaluation of hydrothermal stability. For this study, the physical and chemical properties of TiPCS-derived materials during pyrolysis were characterized via TG-MS, ATR-FTIR, XPS, XRD, and N2 adsorption-desorption isotherms. The pore characteristics and surface areas of TiPCS-derived ceramic powders revealed that the titanium components in TiPCS inhibit and/or reduce the densification of the network structures at elevated temperatures. The network structure of TiPCS-derived, SiC-based membranes showed trends similar to those of TiPCS-derived ceramic powders. The membrane prepared at 750 °C featured reproducibility and attractive selectivities for the PV removal of water or methanol from liquid mixtures.
Qing Wang; Yuta Kawano; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. Development of high-performance sub-nanoporous SiC-based membranes derived from polytitanocarbosilane. Journal of Membrane Science 2019, 598, 117688 .
AMA StyleQing Wang, Yuta Kawano, Liang Yu, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. Development of high-performance sub-nanoporous SiC-based membranes derived from polytitanocarbosilane. Journal of Membrane Science. 2019; 598 ():117688.
Chicago/Turabian StyleQing Wang; Yuta Kawano; Liang Yu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2019. "Development of high-performance sub-nanoporous SiC-based membranes derived from polytitanocarbosilane." Journal of Membrane Science 598, no. : 117688.
Meng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Kazuki Yamamoto; Takahiro Gunji; Toshinori Tsuru. Fine‐tuned, molecular‐composite, organosilica membranes for highly efficient propylene/propane separation via suitable pore size. AIChE Journal 2019, 66, 1 .
AMA StyleMeng Guo, Masakoto Kanezashi, Hiroki Nagasawa, Liang Yu, Kazuki Yamamoto, Takahiro Gunji, Toshinori Tsuru. Fine‐tuned, molecular‐composite, organosilica membranes for highly efficient propylene/propane separation via suitable pore size. AIChE Journal. 2019; 66 (4):1.
Chicago/Turabian StyleMeng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Kazuki Yamamoto; Takahiro Gunji; Toshinori Tsuru. 2019. "Fine‐tuned, molecular‐composite, organosilica membranes for highly efficient propylene/propane separation via suitable pore size." AIChE Journal 66, no. 4: 1.
Sol-gel-derived organosilica membranes with different linking groups consisting of 2 carbon atoms (ethane, ethylene, and acetylene) were fabricated using bis(triethoxysilyl)ethane (BTESE), bis(triethoxysilyl)ethylene (BTESEthy), and bis(triethoxysilyl)acetylene (BTESA). No research group has ever proposed tailoring the microstructure and permeation properties of bridged organosilica membranes as a way to control the bond angles. In this study, however, we found that increases in the Si–O–Si and Si–C–C bond angles contributed to the formation of a loose and uniform structure, which was suggested by the blue shift of Si–O–Si and Si–C–C bonds in the FT-IR spectra. BTESA membranes featured a more open and accessible pore structure, which was suitable for the separation of C3H6/C3H8. The present study provides a novel way to design the microstructure and permeation properties of organosilica membranes via controlling the bond angles in the network structure.
Meng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Kazuki Yamamoto; Takahiro Gunji; Joji Ohshita; Toshinori Tsuru. Tailoring the microstructure and permeation properties of bridged organosilica membranes via control of the bond angles. Journal of Membrane Science 2019, 584, 56 -65.
AMA StyleMeng Guo, Masakoto Kanezashi, Hiroki Nagasawa, Liang Yu, Kazuki Yamamoto, Takahiro Gunji, Joji Ohshita, Toshinori Tsuru. Tailoring the microstructure and permeation properties of bridged organosilica membranes via control of the bond angles. Journal of Membrane Science. 2019; 584 ():56-65.
Chicago/Turabian StyleMeng Guo; Masakoto Kanezashi; Hiroki Nagasawa; Liang Yu; Kazuki Yamamoto; Takahiro Gunji; Joji Ohshita; Toshinori Tsuru. 2019. "Tailoring the microstructure and permeation properties of bridged organosilica membranes via control of the bond angles." Journal of Membrane Science 584, no. : 56-65.
Amine-functionalized organosilica membranes are attracting an increasing amount of attention due to significant potential for the capture of post-combustion CO2. The appealing separation performance of these membranes, however, is generally obtained via compromises to gas permeance. In the present study, a novel, ultramicroporosity-tailored composite (organo)silica membrane with high flux was synthesized via sol-gel co-condensation of a pyrimidine-bridged organoalkoxysilane precursor (BTPP) with a second intrinsically rigid network precursor (BTESE or TEOS). The surface chemistry, ultramicroporosity, and chain-packing state of the initial BTPP-derived membranes can be carefully tuned, which has been verified via Fourier transform infrared (FTIR) spectroscopy, water-contact angle measurement, X-ray diffractions (XRD), and positron annihilation lifetime spectroscopy (PALS). The composite (organo)silica xerogel specimens presented a slightly improved ultramicroporosity with noticeable increases in gas adsorption (CO2 and N2). However, a surprising increase in CO2 permeance (>2000 GPU), with moderate CO2/N2 selectivity (~20), was observed in the resultant composite (organo)silica membranes. Furthermore, gas permeance of the composite membranes far surpassed the values based on Maxwell predictions, indicating a possible molecular-scale dispersion of the composite networks. This novel, porosity-tailored, high-flux membrane holds great potential for use in industrial post-combustion CO2 capture.
Liang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Meng Guo; Norihiro Moriyama; Kenji Ito; Toshinori Tsuru. Tailoring Ultramicroporosity To Maximize CO2 Transport within Pyrimidine-Bridged Organosilica Membranes. ACS Applied Materials & Interfaces 2019, 11, 7164 -7173.
AMA StyleLiang Yu, Masakoto Kanezashi, Hiroki Nagasawa, Meng Guo, Norihiro Moriyama, Kenji Ito, Toshinori Tsuru. Tailoring Ultramicroporosity To Maximize CO2 Transport within Pyrimidine-Bridged Organosilica Membranes. ACS Applied Materials & Interfaces. 2019; 11 (7):7164-7173.
Chicago/Turabian StyleLiang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Meng Guo; Norihiro Moriyama; Kenji Ito; Toshinori Tsuru. 2019. "Tailoring Ultramicroporosity To Maximize CO2 Transport within Pyrimidine-Bridged Organosilica Membranes." ACS Applied Materials & Interfaces 11, no. 7: 7164-7173.
Various types of amine-functionalized silica/organosilica membranes have been developed due to their potentially superior CO2 separation performance. This article reviews the progress made in this field and special attention is paid to elucidating the role of amine type in CO2 separation performance within amine-functionalized silica/organosilica membranes. This review includes a systematic comparison of various organosilica membranes with either unhindered or sterically hindered amines developed in our previous studies. Herein, we thoroughly discuss the structural characterizations and CO2 adsorption/desorption properties of amine-functionalized xerogel powders and CO2 transport/separation performance across the relevant membranes. Future directions for the design and development of high-performance CO2 separation membranes are suggested, and particular attention is paid to the future of activation energies for gas permeation.
Liang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. Role of Amine Type in CO2 Separation Performance within Amine Functionalized Silica/Organosilica Membranes: A Review. Applied Sciences 2018, 8, 1032 .
AMA StyleLiang Yu, Masakoto Kanezashi, Hiroki Nagasawa, Toshinori Tsuru. Role of Amine Type in CO2 Separation Performance within Amine Functionalized Silica/Organosilica Membranes: A Review. Applied Sciences. 2018; 8 (7):1032.
Chicago/Turabian StyleLiang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. 2018. "Role of Amine Type in CO2 Separation Performance within Amine Functionalized Silica/Organosilica Membranes: A Review." Applied Sciences 8, no. 7: 1032.
A facile method for the fabrication of amine-silica membranes with enhanced CO2 separation performance was proposed via the thermally induced liberation of small molecules from quaternary ammonium salt. Quaternary ammonium-silica (QA-SiO1.5) xerogel powders/films were fabricated via sol-gel processing and their thermal stability was systematically studied using thermogravimetric mass spectrometer, Fourier transform infrared, energy dispersive spectroscopy, and positron annihilation lifetime spectroscopy analysis. CO2 sorption performances of QA-SiO1.5 derived xerogel powders were quantitatively compared after assigning their relevant parameters to a dual-mode sorption model. The gas permeation performances of membranes derived from QA-SiO1.5 were evaluated in terms of kinetic diameter and temperature dependence of gas permeance, and activation energy (Ep) required for gas permeation. The results indicate that liberation of the CH3Cl molecules from these membranes significantly improved both CO2 permeation and CO2/N2 separation capabilities. Therefore, the present study provides insight that should be useful in the development of high-performance CO2 separation membranes via the effect of the thermally induced liberation of small molecules. © 2017 American Institute of Chemical Engineers AIChE J, 2017
Liang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Norihiro Moriyama; Toshinori Tsuru; Kenji Ito. Enhanced CO 2 separation performance for tertiary amine‐silica membranes via thermally induced local liberation of CH 3 Cl. AIChE Journal 2017, 64, 1528 -1539.
AMA StyleLiang Yu, Masakoto Kanezashi, Hiroki Nagasawa, Norihiro Moriyama, Toshinori Tsuru, Kenji Ito. Enhanced CO 2 separation performance for tertiary amine‐silica membranes via thermally induced local liberation of CH 3 Cl. AIChE Journal. 2017; 64 (5):1528-1539.
Chicago/Turabian StyleLiang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Norihiro Moriyama; Toshinori Tsuru; Kenji Ito. 2017. "Enhanced CO 2 separation performance for tertiary amine‐silica membranes via thermally induced local liberation of CH 3 Cl." AIChE Journal 64, no. 5: 1528-1539.
Liang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. Fabrication and CO2 permeation properties of amine-silica membranes using a variety of amine types. Journal of Membrane Science 2017, 541, 447 -456.
AMA StyleLiang Yu, Masakoto Kanezashi, Hiroki Nagasawa, Toshinori Tsuru. Fabrication and CO2 permeation properties of amine-silica membranes using a variety of amine types. Journal of Membrane Science. 2017; 541 ():447-456.
Chicago/Turabian StyleLiang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. 2017. "Fabrication and CO2 permeation properties of amine-silica membranes using a variety of amine types." Journal of Membrane Science 541, no. : 447-456.
Liang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Joji Oshita; Akinobu Naka; Toshinori Tsuru. Pyrimidine-bridged organoalkoxysilane membrane for high-efficiency CO 2 transport via mild affinity. Separation and Purification Technology 2017, 178, 232 -241.
AMA StyleLiang Yu, Masakoto Kanezashi, Hiroki Nagasawa, Joji Oshita, Akinobu Naka, Toshinori Tsuru. Pyrimidine-bridged organoalkoxysilane membrane for high-efficiency CO 2 transport via mild affinity. Separation and Purification Technology. 2017; 178 ():232-241.
Chicago/Turabian StyleLiang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Joji Oshita; Akinobu Naka; Toshinori Tsuru. 2017. "Pyrimidine-bridged organoalkoxysilane membrane for high-efficiency CO 2 transport via mild affinity." Separation and Purification Technology 178, no. : 232-241.
Liang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Joji Ohshita; Akinobu Naka; Toshinori Tsuru. Fabrication and Microstructure Tuning of a Pyrimidine-Bridged Organoalkoxysilane Membrane for CO2 Separation. Industrial & Engineering Chemistry Research 2017, 56, 1316 -1326.
AMA StyleLiang Yu, Masakoto Kanezashi, Hiroki Nagasawa, Joji Ohshita, Akinobu Naka, Toshinori Tsuru. Fabrication and Microstructure Tuning of a Pyrimidine-Bridged Organoalkoxysilane Membrane for CO2 Separation. Industrial & Engineering Chemistry Research. 2017; 56 (5):1316-1326.
Chicago/Turabian StyleLiang Yu; Masakoto Kanezashi; Hiroki Nagasawa; Joji Ohshita; Akinobu Naka; Toshinori Tsuru. 2017. "Fabrication and Microstructure Tuning of a Pyrimidine-Bridged Organoalkoxysilane Membrane for CO2 Separation." Industrial & Engineering Chemistry Research 56, no. 5: 1316-1326.