Fabrication of highly permselective silica membranes at ordinary temperatures and pressures using atmospheric-pressure plasma-enhanced chemical vapor deposition

• Project/Area Number: 18K04814
• Research Category: Grant-in-Aid for Scientific Research (C)
• Allocation Type: Multi-year Fund
• Section: 一般
• Review Section: Basic Section 27010:Transport phenomena and unit operations-related
• Research Institution: Hiroshima University
• Principal Investigator: Nagasawa Hiroki 広島大学, 先進理工系科学研究科(工), 助教 (30633937)
• Project Period (FY): 2018-04-01 – 2021-03-31
• Project Status: Completed (Fiscal Year 2020)
• Budget Amount: ¥4,420,000 (Direct Cost: ¥3,400,000、Indirect Cost: ¥1,020,000); Fiscal Year 2020: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000); Fiscal Year 2019: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000); Fiscal Year 2018: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
• Keywords: 大気圧プラズマ / 化学気相蒸着 / 有機無機ハイブリッドシリカ膜 / 分子ふるい膜 / 常温常圧製膜 / 膜分離 / 多孔性シリカ膜 / プラズマCVD

Outline of Final Research Achievements

In this study, we investigated the effects of deposition conditions on the membrane structure and gas permeation characteristics in order to improve the permselectivity of of silica membranes prepared via atmospheric-pressure plasma-enhanced CVD technique. It was found that the size of the sub-nanometer pores to be formed within the silica networks can be controlled by manipulating the molecular structure of the silica precursor (hexamethyldisiloxane (HMDSO) and tetramethyldisiloxane (TMDSO)) and discharge gas composition (diluted gas type (He or Ar) and additional gas (N2) concentration). The resultant membranes showed excellent hydrogen permeation selectivity.

Academic Significance and Societal Importance of the Research Achievements

大気圧プラズマCVD法はシリカ膜を常温常圧で製膜できる技術であり，優れた分子ふるい性を有するシリカ膜を簡便に製膜できる技術である．本研究の最も重要な成果は，製膜条件を変化させることによって，得られる膜の細孔構造や透過特性を制御できることを明らかにした点にある．製膜機構の理解が深まったことで，更なる高透過選択膜の開発が期待される．また，本研究成果は，分離対象に応じて様々な特性を持つシリカ膜を作り分ける可能性を示すものであり，様々な分離系でシリカ膜の実用化を促進する画期的な成果である．

Research Products

• [Journal Article] TiO2 Coatings Via Atmospheric-Pressure Plasma-Enhanced Chemical Vapor Deposition for Enhancing the UV-Resistant Properties of Transparent Plastics (2021)
  • Author(s): Xu Jing、Nagasawa Hiroki、Kanezashi Masakoto、Tsuru Toshinori
  • Journal Title: ACS Omega Volume: 6 Issue: 2 Pages: 1370-1377
  • DOI: 10.1021/acsomega.0c04999
  • Peer Reviewed / Open Access
• [Journal Article] Ultrafast Synthesis of Silica-Based Molecular Sieve Membranes in Dielectric Barrier Discharge at Low Temperature and Atmospheric Pressure (2020)
  • Author(s): Nagasawa Hiroki、Kagawa Takahiko、Noborio Takuji、Kanezashi Masakoto、Ogata Atsushi、Tsuru Toshinori
  • Journal Title: Journal of the American Chemical Society Volume: 143 Issue: 1 Pages: 35-40
  • DOI: 10.1021/jacs.0c09433
  • Peer Reviewed
• [Journal Article] 大気圧プラズマCVD法によるハイブリッドシリカ膜の常温常圧製膜 (2019)
  • Author(s): 長澤 寛規
  • Journal Title: 膜 Volume: 44 Pages: 10-15
  • NAID: 130007593158
  • Peer Reviewed
• [Presentation] Atmospheric-Pressure Plasma-Assisted Synthesis of Silica Membranes for Gas Separation (2021)
  • Author(s): Hiroki Nagasawa
  • Organizer: 2020 Dalian University of Technology-Overseas Partner Universities Series Online Exchange Conference
  • Int'l Joint Research / Invited
• [Presentation] 誘電体バリア放電を用いた大気圧プラズマCVDによるシリカ膜の高速製膜 (2021)
  • Author(s): 長澤 寛規，登尾 拓史，金指 正言，都留 稔了
  • Organizer: 化学工学会第86年会
• [Presentation] 大気圧プラズマCVD 法によるLayered-hybridシリカ膜の作製 (2020)
  • Author(s): 川崎貢功，長澤寛規，金指正言，都留稔了
  • Organizer: 日本膜学会第42年会
• [Presentation] 大気圧プラズマCVD法layered-hybridシリカ膜の気体透過特性 (2020)
  • Author(s): 川崎貢功，長澤寛規，金指正言，都留稔了
  • Organizer: 膜シンポジウム2020
• [Presentation] 大気圧プラズマCVD法による高分子支持体へのシリカ膜の作製と気体透過特性 (2020)
  • Author(s): 川崎貢功，長澤寛規，金指正言，都留稔了
  • Organizer: 化学工学会広島大会2020
• [Presentation] 大気圧プラズマCVDを用いた分子ふるいシリカ膜の気体透過特性と構造制御 (2020)
  • Author(s): 登尾 拓史，長澤 寛規，金指 正言，都留 稔了
  • Organizer: 化学工学会第51回秋季大会
• [Presentation] Plasma-assisted low-temperature fabrication of silica-based membranes for gas separation (2019)
  • Author(s): Hiroki Nagasawa
  • Organizer: 9th International Symposium on Inorganic Membranes
  • Int'l Joint Research / Invited
• [Presentation] Facile synthesis of microporous silica membranes via atmospheric-pressure plasma-enhanced CVD (2019)
  • Author(s): Hiroki Nagasawa, Takuji Noborio, Masakoto Kanezashi, Toshinori Tsuru
  • Organizer: 12th Conference of the Aseanian Membrane Society
  • Int'l Joint Research
• [Presentation] シリカ系多孔膜の大気圧プラズマCVD製膜および気体透過特性 (2019)
  • Author(s): 長澤 寛規
  • Organizer: 第13回 中四国若手CE合宿
  • Invited
• [Presentation] Plasma-assisted low temperature facile synthesis of silica membranes and their application in gas separation (2019)
  • Author(s): Hiroki Nagasawa
  • Organizer: China-Japan Bilateral Symposium on Advanced Membranes
  • Int'l Joint Research / Invited
• [Presentation] 大気圧プラズマCVDシリカ膜の気体透過特性と構造制御 (2019)
  • Author(s): 登尾 拓史，長澤 寛規，金指 正言，都留 稔了
  • Organizer: 日本膜学会第41年会
• [Presentation] 大気圧プラズマCVD条件がシリカ膜の膜構造と気体透過特性に及ぼす影響 (2019)
  • Author(s): 登尾 拓史，長澤 寛規，金指 正言，都留 稔了
  • Organizer: 化学工学会姫路大会2019
• [Presentation] Atmospheric-pressure plasma-enhanced CVD of microporous SiO2 membranes in a direct barrier discharge (2018)
  • Author(s): Hiroki Nagasawa,Takahiko Kagawa, Masakoto Kanezashi, Toshinori Tsuru
  • Organizer: ASCON-IEEChE 2018
  • Int'l Joint Research
• [Presentation] Atmospheric-pressure plasma-enhanced CVD for low-temperature rapid synthesis of silica membranes (2018)
  • Author(s): Hiroki Nagasawa,Takahiko Kagawa, Masakoto Kanezashi, Toshinori Tsuru
  • Organizer: 15th International Conference on Inorganic Membranes
  • Int'l Joint Research
• [Presentation] Plasma-deposition of silica membranesfor gas separation in atmospheric-pressure dielectric barrier discharges (2018)
  • Author(s): Hiroki Nagasawa,Takahiko Kagawa, Masakoto Kanezashi, Toshinori Tsuru
  • Organizer: The 11th Conference of the Aseanian Membrane Society
  • Int'l Joint Research