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Depelopment of microporous TiO2-ZrO2-organic composite membranes with ultra-high permeability for organic solvent liquid phase separation

Research Project

Project/Area Number 20H02505
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 27010:Transport phenomena and unit operations-related
Research InstitutionKobe University

Principal Investigator

Yoshioka Tomohisa  神戸大学, 先端膜工学研究センター, 教授 (50284162)

Co-Investigator(Kenkyū-buntansha) 中川 敬三  神戸大学, 科学技術イノベーション研究科, 准教授 (60423555)
新谷 卓司  神戸大学, 科学技術イノベーション研究科, 特命教授 (90607574)
Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥17,810,000 (Direct Cost: ¥13,700,000、Indirect Cost: ¥4,110,000)
Fiscal Year 2022: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Fiscal Year 2021: ¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2020: ¥9,880,000 (Direct Cost: ¥7,600,000、Indirect Cost: ¥2,280,000)
Keywords膜分離 / ナノろ過 / 逆浸透 / セラミック / キレート配位子 / チタニア / ジルコニア / セラミック膜 / 有機溶剤分離 / 有機キレート配位子 / 分子シミュレーション / ガス分離
Outline of Research at the Start

蒸留法に比べて省エネルギーである,有機溶剤分子混合物の膜分離(超ろ過)法に応用可能な,機械的強度と耐溶剤性を有する新規な複合セラミック膜を開発する.有機キレート分子をTiおよびZr元素に配位させたTiO2とZrO2の複合酸化物膜をゾル-ゲル法により作製し,この有機キレート分子を製膜過程で部分的に除去することにより,金属酸化物中に分離場となる大きさが制御されたサブナノサイズの空隙を形成させる.分子シミュレーションを併用することにより,多孔性無機膜の細孔構造と液体分子の透過/阻止現象の関係を明らかとすることを通じて,超ろ過現象の実証とその基本学理を明らかとする.

Outline of Final Research Achievements

TiO2-ZrO2 composite membranes with organic solvent reverse osmosis performance were successfully prepared by using organic chelating ligands (OCLs), and the pore size and interaction with solvent molecules were controlled by using OCLs with different molecular sizes and structures. The TiO2-ZrO2-OCL membrane showed excellent methanol permeation selectivity in the separation of methanol/toluene mixtures. The permeation mechanism was investigated by permeation tests of several organic solvents, and it was suggested that the interaction between the membrane and solvent molecules as well as the solvent viscosity and the area occupied by solvent molecules had an influence on the permeation mechanism. A new permeation model was proposed in which the difference in surface free energy between the membrane and solvent molecules was considered as the activation energy required for permeation, and the model showed good agreement with experimental results.

Academic Significance and Societal Importance of the Research Achievements

低分子量の有機溶剤分子の液体混合物を相変化することなく「ろ過」できるのかという学術的な問いに対して,多孔性の分離膜を介することで可能であることを明らかとした.その際の選択透過成分の透過性の発現機構に寄与する,分子篩性,膜との親和性,および分離対象分子の物性などに関する知見が得られた.一方,有機溶剤分子混合液体の精製は,蒸発潜熱を必要とする蒸留法によって行われため,一般にエネルギー消費の大きいプロセスである.本研究で開発したセラミックをベースとする多孔性分離膜を用いることで,蒸留法に替わって抜本的な省エネルギー化に繋がる,究極的には気化を伴わない理想的な分離操作の可能性が示された.

Report

(4 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Annual Research Report
  • 2020 Annual Research Report
  • Research Products

    (15 results)

All 2023 2022 2021 2020

All Journal Article (4 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 4 results,  Open Access: 1 results) Presentation (10 results) (of which Int'l Joint Research: 5 results,  Invited: 4 results) Patent(Industrial Property Rights) (1 results)

  • [Journal Article] Organic solvent reverse osmosis characteristics of TiO2-ZrO2-organic chelating ligand (OCL) composite membranes using OCLs with different molecular sizes2023

    • Author(s)
      Kitamura Shunsuke、Yoshioka Tomohisa、Nakagawa Keizo、Kitagawa Tooru、Okamoto Yasunao、Matsuoka Atsushi、Kamio Eiji、Matsuyama Hideto
    • Journal Title

      Separation and Purification Technology

      Volume: 315 Pages: 123576-123576

    • DOI

      10.1016/j.seppur.2023.123576

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Organic solvent permeation characteristics of TiO2-ZrO2 composite nanofiltration membranes prepared using organic chelating ligand to control pore size and surface property2022

    • Author(s)
      Iesako Ryosuke、Yoshioka Tomohisa、Nakagawa Keizo、Shintani Takuji、Matsuoka Atsushi、Kamio Eiji、Matsuyama Hideto
    • Journal Title

      Separation and Purification Technology

      Volume: 297 Pages: 121458-121458

    • DOI

      10.1016/j.seppur.2022.121458

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Graphene quantum dots (GQDs)-assembled membranes with intrinsic functionalized nanochannels for high-performance nanofiltration2021

    • Author(s)
      Yuqing Lin, Qin Shen, Yuki Kawabata, Junpei Segawa, Xingzhong Cao, Kecheng Guan, Titik Istirokhatun, Tomohisa Yoshioka, Hideto Matsuyama
    • Journal Title

      Chemical Engineering Journal

      Volume: 420 Pages: 127602-127602

    • DOI

      10.1016/j.cej.2020.127602

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Gas permeation characteristics of TiO2-ZrO2-aromatic organic chelating ligand (aOCL) composite membranes2020

    • Author(s)
      Takashi Tachibana, Tomohisa Yoshioka, Keizo Nakagawa, Takuji Shintani, Eiji Kamio, Hideto Matsuyama
    • Journal Title

      Membranes

      Volume: 10 Issue: 12 Pages: 388-388

    • DOI

      10.3390/membranes10120388

    • NAID

      120006951635

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] Molecular Dynamics Simulation Study of Liquid Permeation through Nano Scale Pores on Ceramic Membranes2022

    • Author(s)
      Tomohisa Yoshioka, Yuya Ohara, Yuto Ihara, Keizo Nakagawa, Takuji Shintani, Hideto Matsuyama
    • Organizer
      The 16th International Conference on Inorganic Membranes (ICIM-16)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Pore size control of TiO2-ZrO2-organic chelate ligand (OCL) composite membranes for organic solvent nanofiltration (OSN)2022

    • Author(s)
      Shunsuke Kitamuraa, Tomohisa Yoshioka, Keizo Nakagawa, Takuji Shintani, Atsushi Matsuoka, Eiji Kamio, Hideto Matsuyama
    • Organizer
      The 16th International Conference on Inorganic Membranes (ICIM-16)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Molecular transport phenomena and development of microporous ceramic membranes2022

    • Author(s)
      Tomohisa Yoshioka
    • Organizer
      The 13th Conference of the Aseanian Membrane Society (AMS13)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] TiO2-ZrO2-有機キレート配位子(OCL)複合膜における有機溶剤逆浸透分離2022

    • Author(s)
      北村俊介,吉岡朋久,中川敬三,北河享,岡本泰直,松岡淳,神尾英治,松山秀人
    • Organizer
      化学工学会第53回秋季大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 非平衡分子動力学法によるミクロ多孔性膜における 分子輸送現象の解明とセラミック多孔膜の開発2022

    • Author(s)
      吉岡朋久
    • Organizer
      化学工学会第87年会
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] TiO2-ZrO2-有機キレート配位子(OCL)複合膜におけるナノ濾過特性に及ぼすOCLの影響2022

    • Author(s)
      北村俊介,吉岡朋久,中川敬三,新谷卓司,松岡淳,神尾英治,松山秀人
    • Organizer
      化学工学会第87年会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Gas permeation characteristics of microporous TiO2-based ceramic membranes2021

    • Author(s)
      Tomohisa Yoshioka
    • Organizer
      2020 Dalian University of Technology- Overseas Partner Universities Series Online Exchange Conference
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] TiO2-based microporous ceramic-organic chelating ligand (OCL) composite membranes for gas separation and nanofiltration2021

    • Author(s)
      Tomohisa Yoshioka
    • Organizer
      化学工学会第86年会
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] Gas permeation characteristics of TiO2-ZrO2 composite membranes prepared by using aromatic organic chelating ligand (aOCL)2020

    • Author(s)
      Tomohisa Yoshioka, Takashi Tachibana, Keizo Nakagawa, Takuji Shintani, Eiji Kamio, Hideto Matsuyama
    • Organizer
      International Congress on Membranes & Membrane Processes 2020
    • Related Report
      2020 Annual Research Report
    • Int'l Joint Research
  • [Presentation] TiO2-ZrO2-有機キレート配位子(OCL)複合膜の各種有機溶剤透過特性2020

    • Author(s)
      家迫遼介, 吉岡朋久, 中川敬三, 新谷卓司, 神尾英治, 松山秀人
    • Organizer
      化学工学会第51回秋季大会
    • Related Report
      2020 Annual Research Report
  • [Patent(Industrial Property Rights)] ガス分離膜の製造方法、及びガス分離膜2021

    • Inventor(s)
      吉岡朋久,中川敬三,新谷卓司,安成竜輝,家迫遼介,冨澤深雪
    • Industrial Property Rights Holder
      吉岡朋久,中川敬三,新谷卓司,安成竜輝,家迫遼介,冨澤深雪
    • Industrial Property Rights Type
      特許
    • Filing Date
      2021
    • Related Report
      2020 Annual Research Report

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Published: 2020-04-28   Modified: 2024-01-30  

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