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Prof. Dr. Toshinori Tsuru
Department of Chemical Engineering, Hiroshima University, Higashi-Hiroshima, 739-8527, Japan

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0 membrane reactor
0 Inorganic Membranes
0 inorganic/ organic hybrid membranes
0 nano/subnano-porous membranes for gas
0 PV, RO/NF

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membrane reactor
Inorganic Membranes
transport mechanism through nano/subnano-porous membranes

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Journal article
Published: 25 August 2021 in Separation and Purification Technology
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A layered hybrid membrane consisting of an organosilica top layer on a polymeric nanoporous substrate was successfully fabricated using bis(triethoxysilyl)ethane (BTESE)-derived organosilica sols doped with metal ions (Al and Zr). These membranes were applied to the dehydration of aqueous alcohol solutions including methanol (MeOH), ethanol (EtOH) and isopropanol (IPA). Metal-doped BTESE sols and gels were characterized via dynamic light scattering analysis (DLS), Fourier Transform Infrared spectroscopy (FT-IR), X-ray Photoelectron Spectroscopy (XPS), the isotherms of N2 sorption, laser scanning confocal microscopy (LSM), and scanning electron microscopy (SEM). During the dehydration of an IPA solution at 105 °C, the separation factors for Al-BTESE- and Zr-BTESE-derived membranes reached 8,000 and 10,000, respectively, which exceeded the separation factor for undoped BTESE membranes and indicates that doping with metal ions improves the dehydration performance of layered-hybrid membranes. In addition, Zr-BTESE-derived membranes prepared via the rinse method showed water permeance of 1.8 × 10-6 mol m-2 s-1 Pa-1, which is sufficiently high and compares favorably to that of polymer substrates. These membranes also showed a separation factor that was higher than 10,000. Correlations among the permeance ratios for H2O/MeOH, H2O/EtOH, and H2O/IPA were successfully predicted using modified gas translation (mGT) and bimodal pore models.

ACS Style

Takashi Terao; Hiroki Nagasawa; Masakoto Kanezashi; Hiroshi Yanagishita; Toshinori Tsuru. Controlled organosilica networks via metal doping for improved dehydration membranes with layered hybrid structures. Separation and Purification Technology 2021, 119561 .

AMA Style

Takashi Terao, Hiroki Nagasawa, Masakoto Kanezashi, Hiroshi Yanagishita, Toshinori Tsuru. Controlled organosilica networks via metal doping for improved dehydration membranes with layered hybrid structures. Separation and Purification Technology. 2021; ():119561.

Chicago/Turabian Style

Takashi Terao; Hiroki Nagasawa; Masakoto Kanezashi; Hiroshi Yanagishita; Toshinori Tsuru. 2021. "Controlled organosilica networks via metal doping for improved dehydration membranes with layered hybrid structures." Separation and Purification Technology , no. : 119561.

Research article
Published: 18 July 2021 in Applied Organometallic Chemistry
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Organically bridged polysilsesquioxane (PSQ)-based reverse osmosis (RO) membranes have been studied for water desalination. In this work, RO membranes were prepared from tris[3-(triethoxysilyl)propyl]amine (TTESPA), tris[3-(diethoxymethylsilyl)propyl]amine (TDEMSPA), tris[(triethoxysilyl)methyl]amine (TTESMA) tris[(triethoxysilyl)propenyl]amine (TTESP2A), and tris[3-(triethoxysilyl)prop-2-ynyl]amine (TTESP3A) by the sol–gel process and interfacial polymerization. It was found that the TTESPA-derived membranes gave the best RO performance among those prepared. The membrane prepared by the interfacial polymerization of TTESPA showed water permeance and salt rejection of 7.3 × 10−13 m3/m2sPa and 95.6% for 2000 ppm NaCl aqueous solution, respectively, which were higher than those previously reported for a membrane similarly prepared from bis[(triethoxysilyl)propyl]amine (1.4 × 10−13 m3/m2sPa and 93.6%).

ACS Style

Dian Zhang; Masakoto Kanezashi; Toshinori Tsuru; Kazuki Yamamoto; Raku Yakuwa; Takahiro Gunji; Yohei Adachi; Joji Ohshita. Preparation of polysilsesquioxane reverse osmosis membranes for water desalination from tris[(ethoxysilyl)alkyl]amines by sol–gel process and interfacial polymerization. Applied Organometallic Chemistry 2021, e6374 .

AMA Style

Dian Zhang, Masakoto Kanezashi, Toshinori Tsuru, Kazuki Yamamoto, Raku Yakuwa, Takahiro Gunji, Yohei Adachi, Joji Ohshita. Preparation of polysilsesquioxane reverse osmosis membranes for water desalination from tris[(ethoxysilyl)alkyl]amines by sol–gel process and interfacial polymerization. Applied Organometallic Chemistry. 2021; ():e6374.

Chicago/Turabian Style

Dian Zhang; Masakoto Kanezashi; Toshinori Tsuru; Kazuki Yamamoto; Raku Yakuwa; Takahiro Gunji; Yohei Adachi; Joji Ohshita. 2021. "Preparation of polysilsesquioxane reverse osmosis membranes for water desalination from tris[(ethoxysilyl)alkyl]amines by sol–gel process and interfacial polymerization." Applied Organometallic Chemistry , no. : e6374.

Journal article
Published: 27 June 2021 in Separation and Purification Technology
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In this study, nanoporous (pore size: 1.5 nm) and subnanoporous (pore size: 0.42–0.43 nm) organosilica membranes were prepared to accomplish steam recovery via vapor permeation (VP) at high temperatures. These membranes were evaluated under various operating conditions that included high temperatures (80–150 °C), various water mole fractions in the feed stream (0.1–0.9), and various pressures of the feed (130–140 kPa (abs.) or 400 kPa (abs.)) and permeate (~0 kPa (abs.) or 100 kPa (abs.)). A comparison of the performances of nanoporous and subnanoporous membranes clearly showed the advantage of the subnanoporous structure for steam recovery under high temperature. Subnanoporous organosilica membranes showed water permeance of several 10−6 mol/(m2 s Pa) and an H2O/N2 permeance ratio of several hundreds at 150 °C, compared with the results from nanoporous organosilica membranes that were approximately 10−5 mol/(m2 s Pa) and below ten, respectively. Furthermore, subnanoporous organosilica membranes showed a maximum water flux as high as 73 kg/(m2 h) at a transmembrane pressure of 300 kPa during VP. In addition, subnanoporous organosilica membranes showed similar high levels of water permeance for seven binary steam/non-condensable gas (He, H2, CO2, N2, CH4, CF4, SF6) mixtures.

ACS Style

Norihiro Moriyama; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. Steam recovery via nanoporous and subnanoporous organosilica membranes: The effects of pore structure and operating conditions. Separation and Purification Technology 2021, 275, 119191 .

AMA Style

Norihiro Moriyama, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. Steam recovery via nanoporous and subnanoporous organosilica membranes: The effects of pore structure and operating conditions. Separation and Purification Technology. 2021; 275 ():119191.

Chicago/Turabian Style

Norihiro Moriyama; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2021. "Steam recovery via nanoporous and subnanoporous organosilica membranes: The effects of pore structure and operating conditions." Separation and Purification Technology 275, no. : 119191.

Journal article
Published: 03 June 2021 in Separation and Purification Technology
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TiO2-ZrO2 nanofiltration (NF) membranes with different Ti/Zr molar ratios were evaluated for stability in hot water and strong acid/alkaline solutions. Each treatment condition was followed by an evaluation of the NF performance at 25 °C (ΔP = 1.0 MPa, pH 7). In hydrothermal tests in water for 100 h, all TiO2-ZrO2 membranes were stable. On the other hand, under corrosion tests at pH 2 the membranes with Ti-rich compositions (Ti/Zr= 10/0, 9/1, 7/3) were less stable than those with less Ti in the composition (Ti/Zr= 5/5, 3/7, 1/9, 0/10), which could be ascribed to the high solubility of Ti in strong acid, and indicates that Ti-rich membranes will provide inadequate corrosion resistance against strong acids. Moreover, all membranes showed high corrosion resistance in alkaline solutions at pH 13. Therefore, TiO2-ZrO2 (5/5, 3/7, 1/9, 0/10) membranes proved sufficiently stable both in strong acid and in strong alkaline solutions.

ACS Style

Sofiatun Anisah; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. Effect of the Ti/Zr ratio on the hydrothermal and chemical stability of TiO2-ZrO2 nanofiltration membranes. Separation and Purification Technology 2021, 274, 119060 .

AMA Style

Sofiatun Anisah, Masakoto Kanezashi, Hiroki Nagasawa, Toshinori Tsuru. Effect of the Ti/Zr ratio on the hydrothermal and chemical stability of TiO2-ZrO2 nanofiltration membranes. Separation and Purification Technology. 2021; 274 ():119060.

Chicago/Turabian Style

Sofiatun Anisah; Masakoto Kanezashi; Hiroki Nagasawa; Toshinori Tsuru. 2021. "Effect of the Ti/Zr ratio on the hydrothermal and chemical stability of TiO2-ZrO2 nanofiltration membranes." Separation and Purification Technology 274, no. : 119060.

Research article
Published: 02 June 2021 in Industrial & Engineering Chemistry Research
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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.

ACS Style

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 Style

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 (23):8527-8537.

Chicago/Turabian Style

Keita 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.

Research article
Published: 06 May 2021 in ACS Applied Materials & Interfaces
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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.

ACS Style

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 Style

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 (19):23247-23259.

Chicago/Turabian Style

Ufafa 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.

Journal article
Published: 04 May 2021 in AIChE Journal
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A fluorine‐SiO2 membrane was prepared using triethoxyfluorosilane (TEFS) as a Si precursor, and its hydrothermal stability was evaluated. The TEFS membrane calcined at 750°C had fewer Si‐OH and Si‐F groups in its network structure and showed H2 permeance that was greater than 10−6 mol m−2 s−1 Pa−1 with H2/N2 and N2/SF6 permeance ratios of 10 and 210, respectively. This membrane performance was relatively stable under the temperature (< 500°C) used for steam treatment, regardless of the steam partial pressure (30, 90 kPa). On the other hand, when the steam treatment temperature was increased beyond 500°C, gas permeance decreased significantly and the membrane became highly selective for He and H2 over smaller molecules (He/N2: > 600, H2/N2: > 100). The relationship between the activation energy of H2 and the permeance ratios (He/H2, He/H2O, H2/H2O) of a TEFS‐derived membrane under steam treatment higher than 600°C resulted in a network pore size that approximated in conventional microporous SiO2 membranes.

ACS Style

Masakoto Kanezashi; Naoya Hataoka; Rana Ikram; Hiroki Nagasawa; Toshinori Tsuru. Hydrothermal stability of fluorine‐induced microporous silica membranes: Effect of steam treatment conditions. AIChE Journal 2021, e17292 .

AMA Style

Masakoto Kanezashi, Naoya Hataoka, Rana Ikram, Hiroki Nagasawa, Toshinori Tsuru. Hydrothermal stability of fluorine‐induced microporous silica membranes: Effect of steam treatment conditions. AIChE Journal. 2021; ():e17292.

Chicago/Turabian Style

Masakoto Kanezashi; Naoya Hataoka; Rana Ikram; Hiroki Nagasawa; Toshinori Tsuru. 2021. "Hydrothermal stability of fluorine‐induced microporous silica membranes: Effect of steam treatment conditions." AIChE Journal , no. : e17292.

Paper
Published: 09 April 2021 in Molecular Systems Design & Engineering
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This work demonstrates that conversion of ligand–Si–Zr composite with polymer-like gas permeation behviour into rigid structures displaying silica-like permeation behaviour is easily achieved by a thermal radical crosslinking.

ACS Style

Sulaiman Oladipo Lawal; Hiroki Nagasawa; Toshinori Tsuru; Masakoto Kanezashi. Facile development of microstructure-engineered, ligand-chelated SiO2–ZrO2 composite membranes for molecular separations. Molecular Systems Design & Engineering 2021, 6, 429 -444.

AMA Style

Sulaiman Oladipo Lawal, Hiroki Nagasawa, Toshinori Tsuru, Masakoto Kanezashi. Facile development of microstructure-engineered, ligand-chelated SiO2–ZrO2 composite membranes for molecular separations. Molecular Systems Design & Engineering. 2021; 6 (6):429-444.

Chicago/Turabian Style

Sulaiman Oladipo Lawal; Hiroki Nagasawa; Toshinori Tsuru; Masakoto Kanezashi. 2021. "Facile development of microstructure-engineered, ligand-chelated SiO2–ZrO2 composite membranes for molecular separations." Molecular Systems Design & Engineering 6, no. 6: 429-444.

Journal article
Published: 11 March 2021 in Membranes
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A new polyhedral oligomeric silsesquioxane (POSS) designed with eight –(CH2)3–NH–(CH2)2–NH2 groups (PNEN) at its apexes was used as nanocomposite uploading into 1,2-bis(triethoxysilyl)ethane (BTESE)-derived organosilica to prepare mixed matrix membranes (MMMs) for gas separation. The mixtures of BTESE-PNEN were uniform with particle size of around 31 nm, which is larger than that of pure BTESE sols. The characterization of thermogravimetric (TG) and gas permeance indicates good thermal stability. A similar amine-contained material of 3-aminopropyltriethoxysilane (APTES) was doped into BTESE to prepare hybrid membranes through a copolymerized strategy as comparison. The pore size of the BTESE-PNEN membrane evaluated through a modified gas-translation model was larger than that of the BTESE-APTES hybrid membrane at the same concentration of additions, which resulted in different separation performance. The low values of Ep(CO2)-Ep(N2) and Ep(N2) for the BTESE-PNEN membrane at a low concentration of PNEN were close to those of copolymerized BTESE-APTES-related hybrid membranes, which illustrates a potential CO2 separation performance by using a mixed matrix membrane strategy with multiple amine POSS as particles.

ACS Style

Xiuxiu Ren; Masakoto Kanezashi; Meng Guo; Rong Xu; Jing Zhong; Toshinori Tsuru. Multiple Amine-Contained POSS-Functionalized Organosilica Membranes for Gas Separation. Membranes 2021, 11, 194 .

AMA Style

Xiuxiu Ren, Masakoto Kanezashi, Meng Guo, Rong Xu, Jing Zhong, Toshinori Tsuru. Multiple Amine-Contained POSS-Functionalized Organosilica Membranes for Gas Separation. Membranes. 2021; 11 (3):194.

Chicago/Turabian Style

Xiuxiu Ren; Masakoto Kanezashi; Meng Guo; Rong Xu; Jing Zhong; Toshinori Tsuru. 2021. "Multiple Amine-Contained POSS-Functionalized Organosilica Membranes for Gas Separation." Membranes 11, no. 3: 194.

Journal article
Published: 06 March 2021 in Separation and Purification Technology
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Perfluorosulfonic acid membranes perform water vapor permeation at a high level. Few studies, however, have described the water vapor permeance of dehumidification membranes. In this study, therefore, perfluorosulfonic acid capillary membranes used in commercial membrane dehumidifiers were examined to clarify the measurement conditions that are used to evaluate water vapor permeation performance. The measurement conditions include an operating temperature of 10–40 °C, a feed gas relative humidity (RH) of 0–90%, and a total feed side pressure of 0.2 MPaG. Water vapor permeation was evaluated by measuring slight changes in the RH of sweep gas on the permeate sides using countercurrent modules with an effective membrane length of 80 mm. Regarding the RH of the feed gas, the difference between feed-in and sweep-in RH was set to 20% or less to minimize the water vapor pressure difference across the membranes. The water vapor flux was higher under high operating temperatures and high levels of feed gas RH. On the other hand, the water vapor permeance increased with increasing feed gas RH but decreased with increasing operating temperature. Under conditions of 10 °C and feed-in RH of 90%, a high water vapor permeance of 1.6 × 10−5 mol/(m2 s Pa) was obtained. To verify the dependence of water vapor permeation performance on the feed gas species used, measurements were carried out using air, N2, He, and CO2 as the feed gases. The water vapor permeation performance showed no dependence on feed gases of air, N2, or He, but permeation was decreased when CO2 gas was used.

ACS Style

Sho Suzuki; Nobuyoshi Shoji; Toshinori Tsuru. Performance evaluation of water vapor permeation through perfluorosulfonic acid capillary membranes. Separation and Purification Technology 2021, 266, 118508 .

AMA Style

Sho Suzuki, Nobuyoshi Shoji, Toshinori Tsuru. Performance evaluation of water vapor permeation through perfluorosulfonic acid capillary membranes. Separation and Purification Technology. 2021; 266 ():118508.

Chicago/Turabian Style

Sho Suzuki; Nobuyoshi Shoji; Toshinori Tsuru. 2021. "Performance evaluation of water vapor permeation through perfluorosulfonic acid capillary membranes." Separation and Purification Technology 266, no. : 118508.

Research article
Published: 23 February 2021 in Materials Chemistry Frontiers
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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.

ACS Style

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 Style

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 (7):3029-3042.

Chicago/Turabian Style

Ufafa 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.

Journal article
Published: 01 February 2021 in AIChE Journal
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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.

ACS Style

Norihiro Moriyama; Yuta Kawano; Qing Wang; Ryota Inoue; Meng Guo; Makoto Yokoji; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation. AIChE Journal 2021, 67, e17223 .

AMA Style

Norihiro Moriyama, Yuta Kawano, Qing Wang, Ryota Inoue, Meng Guo, Makoto Yokoji, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation. AIChE Journal. 2021; 67 (7):e17223.

Chicago/Turabian Style

Norihiro Moriyama; Yuta Kawano; Qing Wang; Ryota Inoue; Meng Guo; Makoto Yokoji; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2021. "Pervaporation via silicon‐based membranes: Correlation and prediction of performance in pervaporation and gas permeation." AIChE Journal 67, no. 7: e17223.

Review article
Published: 17 January 2021 in Separation and Purification Technology
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Acetic acid is an essential intermediate chemical and belongs to the top 50 commodities of the chemical industry. Dehydration of acetic acid/water mixture is an indispensable process for the final acetic acid product. As an effective alternative technique for energy-intensive distillation, pervaporation is getting significant attention for this target separation due to its high efficiency, low energy requirements, and eco-friendly nature. In the present review, the advances in pervaporation membranes, especially polymeric membranes, composite membranes, zeolite membranes, and sol–gel derived ceramic membranes are covered for dehydration of acetic acid/water mixture. The developed strategies to overcome the tradeoff between membrane hydrophilicity and acid resistance are discussed for each kind of membrane with a particular focus on tuning framework Si/Al ratio and Al atom spatial distribution of zeolite membranes, and development of hybrid silica membranes. Thus, pervaporation membranes performance is described along with future prospects and challenges for their commercialization as acid-resistant membranes. In addition to this, we have critically discussed the use of hollow fiber technology for the dehydration of acetic acid and stressed the need of acid-resistant membranes for esterification reactions to improve the yield of the final product.

ACS Style

Waseem Raza; Jixuan Wang; Jianhua Yang; Toshinori Tsuru. Progress in pervaporation membranes for dehydration of acetic acid. Separation and Purification Technology 2021, 262, 118338 .

AMA Style

Waseem Raza, Jixuan Wang, Jianhua Yang, Toshinori Tsuru. Progress in pervaporation membranes for dehydration of acetic acid. Separation and Purification Technology. 2021; 262 ():118338.

Chicago/Turabian Style

Waseem Raza; Jixuan Wang; Jianhua Yang; Toshinori Tsuru. 2021. "Progress in pervaporation membranes for dehydration of acetic acid." Separation and Purification Technology 262, no. : 118338.

Research article
Published: 06 January 2021 in ACS Omega
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Herein, TiO2 coatings were deposited on photodegradable polymers for protection from UV irradiation using the atmospheric-pressure plasma-enhanced chemical vapor deposition (AP-PECVD) technique. Polymethylmethacrylate (PMMA) and polycarbonate (PC) substrates were coated with titanium tetraisopropoxide as the precursor in an open-air atmospheric-pressure nonequilibrium argon plasma jet. The AP-PECVD-derived TiO2 coatings exhibited good adhesion to PMMA and PC. The TiO2 coatings could shield more than 99% of UV light in the wavelength range of 200–300 nm, without affecting the transmittance of visible light. UV irradiation tests on polymer films demonstrated that the degradation rates of PMMA and PC were significantly reduced by one-tenth after they were coated with TiO2 films.

ACS Style

Jing Xu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. TiO2 Coatings Via Atmospheric-Pressure Plasma-Enhanced Chemical Vapor Deposition for Enhancing the UV-Resistant Properties of Transparent Plastics. ACS Omega 2021, 6, 1370 -1377.

AMA Style

Jing Xu, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. TiO2 Coatings Via Atmospheric-Pressure Plasma-Enhanced Chemical Vapor Deposition for Enhancing the UV-Resistant Properties of Transparent Plastics. ACS Omega. 2021; 6 (2):1370-1377.

Chicago/Turabian Style

Jing Xu; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2021. "TiO2 Coatings Via Atmospheric-Pressure Plasma-Enhanced Chemical Vapor Deposition for Enhancing the UV-Resistant Properties of Transparent Plastics." ACS Omega 6, no. 2: 1370-1377.

Rapid communication
Published: 29 December 2020 in Journal of the American Chemical Society
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Microporous silica membranes have shown promise as potential candidates for energy-efficient chemical separation. Herein, we report the ultrafast synthesis of silica membranes, on the order of minutes, in atmospheric-pressure, low-temperature plasma. Direct deposition in the discharge region of atmospheric-pressure plasma enables the immediate formation of a thin silica layer on a porous substrate. The plasma-deposited layer had a thickness of ∼13 nm and was confined to the immediate surface of the substrate. With an increase in deposition temperature, we observed an increase in the inorganic nature of the plasma-deposited layer and simultaneous improvement in the membrane performance. Consequently, the resulting membranes exhibited outstanding permeance for small-sized gas molecules, such as H2 (>10–6 mol m–2 s–1 Pa–1), with a high H2/SF6 permeance ratio of ∼6300, providing a nonthermal alternative for the fabrication of silica-based membranes.

ACS Style

Hiroki Nagasawa; Takahiko Kagawa; Takuji Noborio; Masakoto Kanezashi; Atsushi Ogata; Toshinori Tsuru. Ultrafast Synthesis of Silica-Based Molecular Sieve Membranes in Dielectric Barrier Discharge at Low Temperature and Atmospheric Pressure. Journal of the American Chemical Society 2020, 143, 35 -40.

AMA Style

Hiroki Nagasawa, Takahiko Kagawa, Takuji Noborio, Masakoto Kanezashi, Atsushi Ogata, Toshinori Tsuru. Ultrafast Synthesis of Silica-Based Molecular Sieve Membranes in Dielectric Barrier Discharge at Low Temperature and Atmospheric Pressure. Journal of the American Chemical Society. 2020; 143 (1):35-40.

Chicago/Turabian Style

Hiroki Nagasawa; Takahiko Kagawa; Takuji Noborio; Masakoto Kanezashi; Atsushi Ogata; Toshinori Tsuru. 2020. "Ultrafast Synthesis of Silica-Based Molecular Sieve Membranes in Dielectric Barrier Discharge at Low Temperature and Atmospheric Pressure." Journal of the American Chemical Society 143, no. 1: 35-40.

Journal article
Published: 18 December 2020 in IEEE Transactions on Nanotechnology
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Starting from room temperature (27°C), graphene oxide (GO) was annealed stepwise at 100°C, 200°C and 300°C and detailed structural characterizations like FTIR (Fourier transform infrared spectroscopy), XPS (X-ray photoelectron spectroscopy), XRD (X-ray powder diffraction) and Raman spectroscopy revealed that with increase in temperature, transformation from GO to rGO (reduced graphene oxide) took place and complete conversion was achieved at 300°C. With increase in temperature, the functional groups like epoxy, ether, carbonyl and carboxyl were gradually reduced and at 300°C, only the hydroxyl group became dominant. The gas sensing study was carried out using NH3 and alcohols in the concentration range of 125 ppb-700 ppm. It was observed that for lower ppm (5-50 ppm) the GO based sensors offered better selectivity towards NH3, while rGO exhibited better NH3 selectivity at higher concentrations (200-700 ppm). Possibly, presence of hydroxyl group is favorable for NH3 adsorption and therefore NH3 selectivity is better in rGO particularly at high concentrations. On the other hand, at low NH3 concentrations, presence of various types of functional groups in GO gives a resultant selectivity which is better compared to that of rGO.

ACS Style

Indranil Maity; Hiroki Nagasawa; Toshinori Tsuru; Partha Bhattacharyya. Correlation Between Ammonia Selectivity and Temperature Dependent Functional Group Tuning of GO. IEEE Transactions on Nanotechnology 2020, 20, 129 -136.

AMA Style

Indranil Maity, Hiroki Nagasawa, Toshinori Tsuru, Partha Bhattacharyya. Correlation Between Ammonia Selectivity and Temperature Dependent Functional Group Tuning of GO. IEEE Transactions on Nanotechnology. 2020; 20 (99):129-136.

Chicago/Turabian Style

Indranil Maity; Hiroki Nagasawa; Toshinori Tsuru; Partha Bhattacharyya. 2020. "Correlation Between Ammonia Selectivity and Temperature Dependent Functional Group Tuning of GO." IEEE Transactions on Nanotechnology 20, no. 99: 129-136.

Paper
Published: 17 November 2020 in RSC Advances
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In the present study, SiC particles derived mesoporous membrane was discovered and applied to membrane reactor for H2SO4 decomposition. The reaction equilibrium was moved the to the product side by membrane reactor with extraction at 600 °C.

ACS Style

Xin Yu; Qing Wang; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. SiC mesoporous membranes for sulfuric acid decomposition at high temperatures in the iodine–sulfur process. RSC Advances 2020, 10, 41883 -41890.

AMA Style

Xin Yu, Qing Wang, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. SiC mesoporous membranes for sulfuric acid decomposition at high temperatures in the iodine–sulfur process. RSC Advances. 2020; 10 (68):41883-41890.

Chicago/Turabian Style

Xin Yu; Qing Wang; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2020. "SiC mesoporous membranes for sulfuric acid decomposition at high temperatures in the iodine–sulfur process." RSC Advances 10, no. 68: 41883-41890.

Journal article
Published: 11 November 2020 in Journal of Membrane Science
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To examine the prospect of a future application of organosilica membranes to steam recovery under hydrothermal conditions, we proposed a novel concept that involved a hydrothermally stable intermediate layer derived from colloidal 1,2-bis(triethoxysilyl)ethane (BTESE) sols with a BTESE-derived separation top layer. In this work, a BTESE-derived nanoporous intermediate layer (i-BTESE) was prepared from a BTESE-derived colloidal sol without pinholes or cracks, and then a BTESE-derived sub-nanoporous separation layer was formed on the i-BTESE to obtain a BTESE/i-BTESE membrane. The BTESE/i-BTESE membrane showed excellent water permeance as high as 5 × 10-6 mol/(m2 s Pa), and a high level of permeance was maintained for as long as 361 h at 200°C under vapor pressure of 200 kPa (abs.). In addition, the membrane achieved an H2O/N2 permeance ratio that reached as high as 350 even after 361 h. On the other hand, the permeance of a conventional BTESE-derived membrane that used a silica-zirconia intermediate layer (BTESE/i-SiO2-ZrO2) decreased gradually, which suggested a degradation of the BTESE/i-SiO2-ZrO2 membrane. The high and stable performance of the BTESE/i-BTESE membrane confirmed the proposed concept whereby a hydrothermally stable intermediate layer could significantly improve the hydrothermal stability that is required in order to use organosilica membranes in steam recovery.

ACS Style

Norihiro Moriyama; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. Improved performance of organosilica membranes for steam recovery at moderate-to-high temperatures via the use of a hydrothermally stable intermediate layer. Journal of Membrane Science 2020, 620, 118895 .

AMA Style

Norihiro Moriyama, Hiroki Nagasawa, Masakoto Kanezashi, Toshinori Tsuru. Improved performance of organosilica membranes for steam recovery at moderate-to-high temperatures via the use of a hydrothermally stable intermediate layer. Journal of Membrane Science. 2020; 620 ():118895.

Chicago/Turabian Style

Norihiro Moriyama; Hiroki Nagasawa; Masakoto Kanezashi; Toshinori Tsuru. 2020. "Improved performance of organosilica membranes for steam recovery at moderate-to-high temperatures via the use of a hydrothermally stable intermediate layer." Journal of Membrane Science 620, no. : 118895.

Review
Published: 03 November 2020 in Journal of Membrane Science
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The separation of organic liquid mixtures by organic solvent reverse osmosis (OSRO) technology is promising owing to the high energy-efficiency. This article presents an overview of the endeavors made in the OSRO separation of organic liquid mixtures. First, the sub-nanometer separation characteristic of OSRO is introduced, and compared with pervaporation and organic solvent nanofiltration. Next, the mixtures of interest which may benefit from OSRO technology such as polar/nonpolar mixtures and their application scenarios are presented. The energy evaluation of OSRO, pervaporation, and distillation processes is also performed, highlighting the energy conservation feature of OSRO process. Subsequently, the OSRO membranes developed to date are comprehensively reviewed in term of their membrane materials, diving into organic (mainly cellulose types, polyethylene, polyamide, perfluoropolymer), inorganic (carbon molecular sieves, silica, zeolite), and composite (polymers of intrinsic microporosity-1/AlOx) materials. The OSRO separation performances of the developed membranes are summarized and compared in term of flux and separation factor. Finally, we provide perspectives regarding the challenges and state the concluding remarks, in the hope that this review will inspire future studies to address efficient OSRO separations.

ACS Style

Cuijing Liu; Guanying Dong; Toshinori Tsuru; Hideto Matsuyama. Organic solvent reverse osmosis membranes for organic liquid mixture separation: A review. Journal of Membrane Science 2020, 620, 118882 .

AMA Style

Cuijing Liu, Guanying Dong, Toshinori Tsuru, Hideto Matsuyama. Organic solvent reverse osmosis membranes for organic liquid mixture separation: A review. Journal of Membrane Science. 2020; 620 ():118882.

Chicago/Turabian Style

Cuijing Liu; Guanying Dong; Toshinori Tsuru; Hideto Matsuyama. 2020. "Organic solvent reverse osmosis membranes for organic liquid mixture separation: A review." Journal of Membrane Science 620, no. : 118882.

Paper
Published: 02 November 2020 in Journal of Materials Chemistry A
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Weak van der Waals forces between anisotropic carbon layers doped into a SiO2–ZrO2 matrix allow reversible pressure-induced switching of CO2 between monolayer and multilayer adsorption.

ACS Style

Sulaiman Oladipo Lawal; Liang Yu; Hiroki Nagasawa; Toshinori Tsuru; Masakoto Kanezashi. A carbon–silica–zirconia ceramic membrane with CO2 flow-switching behaviour promising versatile high-temperature H2/CO2 separation. Journal of Materials Chemistry A 2020, 8, 23563 -23573.

AMA Style

Sulaiman Oladipo Lawal, Liang Yu, Hiroki Nagasawa, Toshinori Tsuru, Masakoto Kanezashi. A carbon–silica–zirconia ceramic membrane with CO2 flow-switching behaviour promising versatile high-temperature H2/CO2 separation. Journal of Materials Chemistry A. 2020; 8 (44):23563-23573.

Chicago/Turabian Style

Sulaiman Oladipo Lawal; Liang Yu; Hiroki Nagasawa; Toshinori Tsuru; Masakoto Kanezashi. 2020. "A carbon–silica–zirconia ceramic membrane with CO2 flow-switching behaviour promising versatile high-temperature H2/CO2 separation." Journal of Materials Chemistry A 8, no. 44: 23563-23573.